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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Organic contamination detection for isotopic analysis of water by laser spectroscopy

Hydrogen and oxygen stable isotope ratios (δ 2 H, δ 17 O, and δ 18 O values) are commonly used tracers of water. These ratios can be measured by isotope ratio infrared spectroscopy (IRIS). However, IRIS approaches are prone to errors induced by organic compounds present in plant, soil, and natural water samples. A novel approach using 17 O-excess values has shown promise for flagging spectrally contaminated plant samples during IRIS analysis. A systematic assessment of this flagging system is needed to prove it useful. Errors induced by methanol and ethanol water mixtures on measured IRIS and isotope ratio mass spectrometry (IRMS) results were evaluated. For IRIS analyses both liquid- and vapour-mode (via direct vapour equilibration) methods are used. The δ 2 H, δ 17 O, and δ 18 O values were measured and compared with known reference values to determine the errors induced by methanol and ethanol contamination. In addition, the 17 O-excess contamination detection approach was tested. This is a post-processing detection tool for both liquid and vapour IRIS triple-isotope analyses, utilizing calculated 17 O-excess values to flag contaminated samples. Organic contamination induced significant errors in IRIS results, not seen in IRMS results. Methanol caused larger errors than ethanol. Results from vapour-IRIS analyses had larger errors than those from liquid-IRIS analyses. The 17 O-excess approach identified methanol driven error in liquid- and vapour-mode IRIS samples at levels where isotope results became unacceptably erroneous. For ethanol contaminated samples, a mix of erroneous and correct flagging occurred with the 17 O-excess method. Here our results indicate that methanol is the more problematic contaminant for data corruption. The 17 O-excess method was therefore useful for data quality control. Organic contamination caused significant errors in IRIS stable isotope results. These errors were larger during vapour analyses than during liquid IRIS analyses, and larger for methanol than ethanol contamination. The 17 O-excess method is highly sensitive for detecting narrowband (methanol) contamination error in vapour and liquid analysis modes in IRIS.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2025

Leveraging artificial intelligence and advanced food processing techniques for enhanced food safety, quality, and security: a comprehensive review

Artificial intelligence is emerging as a transformative force in addressing the multifaceted challenges of food safety, food quality, and food security. This review synthesizes advancements in AI-driven technologies, such as machine learning, deep learning, natural language processing, and computer vision, and their applications across the food supply chain, based on a comprehensive analysis of literature published from 1990 to 2024. AI enhances food safety through real-time contamination detection, predictive risk modeling, and compliance monitoring, reducing public health risks. It improves food quality by automating defect detection, optimizing shelf-life predictions, and ensuring consistency in taste, texture, and appearance. Furthermore, AI addresses food security by enabling resource-efficient agriculture, yield forecasting, and supply chain optimization to ensure the availability and accessibility of nutritious food resources. This review also highlights the integration of AI with advanced food processing techniques such as high-pressure processing, ultraviolet treatment, pulsed electric fields, cold plasma, and irradiation, which ensure microbial safety, extend shelf life, and enhance product quality. Additionally, the integration of AI with emerging technologies such as the Internet of Things, blockchain, and AI-powered sensors enables proactive risk management, predictive analytics, and automated quality control. By examining these innovations' potential to enhance transparency, efficiency, and decision-making within food systems, this review identifies current research gaps and proposes strategies to address barriers such as data limitations, model generalizability, and ethical concerns. These insights underscore the critical role of AI in advancing safer, higher-quality, and more secure food systems, guiding future research and fostering sustainable food systems that benefit public health and consumer trust.

AI↗
DOE OSTI2019

Preparing the FUSRAP Colonie Interim Storage Site for Transfer Back to the US Department of Energy Office of Legacy Management - 19215

The Formerly Utilized Sites Remedial Action Program (FUSRAP) Colonie Interim Storage Site was transferred from the US Department of Energy (US DOE) to the US Army Corps of Engineers (USACE) in 1997. The USACE initiated remediation efforts at the Site under FUSRAP. The Site was separated into three distinct operable units (OU) to more efficiently manage the remedial process: 1) Groundwater OU, 2) Main Site Soils OU, and 3) Vicinity Property OU. The USACE has completed remedial actions at each of these three OUs and has advanced the OU remedies at the Site to the long-term stewardship stage to be executed by the US DOE Office of Legacy Management (LM). The US DOE LM is the current real property owner of record of the Colonie Main Site. A summary of each OU and the activities needed to prepare for site transfer follows: OU 1 - USACE issued the Colonie Groundwater OU Record of Decision (ROD) (USACE 2010a) on April 9, 2010. The Groundwater ROD remedy is monitored natural attenuation (MNA) and long-term monitoring (LTM) of groundwater after source removal completion. Results of groundwater monitoring indicate reductions in concentrations of contaminants of concern (COC). Based on the marked progress to date, USACE has optimized the groundwater LTM program (USACE, 2014) by reducing the well network, sampling frequency, and analytical parameters, and by abandoning wells that are no longer needed. A Groundwater ROD Five-Year Review report was submitted to the New York State Department of Environmental Conservation (NYSDEC) for review in 2018. NYSDEC agreed that MNA is still an appropriate remedial method although it is progressing at a slower rate than predicted. OU 2 - From 1999 to 2007, USACE completed the large-scale removal of soil at the Main Site, which included the adjacent Town of Colonie Vicinity Property. Radioactively contaminated soil along with accessible metals-contaminated soil and soil containing volatile organic compounds (VOC) were removed during this effort. A total of 103,402 cubic meters (m{sup 3}) of soil was excavated and disposed offsite. On March 26, 2015, USACE signed the Main Site Soils OU ROD (USACE, 2015a). The ROD remedy included provisions for Land Use Controls (LUC) consisting of institutional controls (IC) through an Environmental Easement for management of three small and discrete inaccessible locations within three of the 27 Final Status Survey units of the Main Site. The Environmental Easement provides a means of protection based on both current and future land use by placing restrictions on soil excavation and reuse. The easement and a supporting Site Management Plan (SMP) will be finalized by LM in coordination with NYSDEC. OU 3 - the Vicinity Property OU ROD was signed on 20 September 2017. This ROD declared No Action (NA) for dust and No Further Action (NFA) for soil and other media for the Vicinity Properties. Prior to the ROD, USACE performed dust sampling and other characterization activities at representative commercial and residential Vicinity Property locations. These efforts were reported in the Colonie FUSRAP Site Vicinity Property Operable Unit Remedial Investigation Summary Report (USACE, 2016). A Site Closeout Report (SCOR) was issued to NYSDEC and approved in 2018. The approval of this report starts the transfer process back to the LM. Ongoing and future transfer activities include records retention and management, preparation and filing of real estate records, physical site management (fencing, landscape maintenance, well abandonment) and coordination with state regulators and LM staff. This presentation is intended to make all stakeholders aware of the necessary steps for site transfer from the USACE back to the LM. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

2018 Postclosure Groundwater Monitoring and Inspection Report, Central Nevada Test Area, Nevada, Subsurface Corrective Action Unit 443

This report presents the groundwater monitoring data collected by the U.S. Department of Energy (DOE) Office of Legacy Management (LM) from the Central Nevada Test Area (CNTA), Nevada, Site, Subsurface Corrective Action Unit (CAU) 443 in Nye County, Nevada (Figure 1). CNTA is the site of an underground nuclear test in 1968 that resulted in residual contamination near the detonation depth of 3200 feet (ft); the contamination requires long-term monitoring. Responsibility for the environmental restoration and long-term monitoring was transferred from DOE’s National Nuclear Security Administration, Nevada Field Office, to LM on October 1, 2006. The environmental restoration and site closure process were completed in 2015 in accordance with the amended Federal Facility Agreement and Consent Order (FFACO) (FFACO 1996, as amended) and all applicable Nevada Division of Environmental Protection (NDEP) policies and regulations. The Closure Report, Central Nevada Test Area, Subsurface Corrective Action, Unit 443 (DOE 2018a), also called the Closure Report, originally was completed in January 2016 and revised in October 2018; it describes LM’s plan for long-term postclosure monitoring. This includes monitoring of the radioisotopes of interest and water elevations, inspecting the site and maintaining the institutional controls (ICs), evaluating and reporting data, and documenting the site’s records and data management processes (DOE 2018a).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

2016 Postclosure Groundwater Monitoring and Inspection Report, Central Nevada Test Area, Nevada, Subsurface Corrective Action Unit 443

This report presents the groundwater monitoring data collected by the U.S. Department of Energy (DOE) Office of Legacy Management (LM) from the Central Nevada Test Area (CNTA), Nevada, Site, Subsurface Corrective Action Unit (CAU) 443 in Nye County, Nevada (Figure 1). The site was the location of an underground nuclear test in 1968, which resulted in residual contamination at and near the detonation depth of approximately 3200 feet (ft) below ground surface (bgs) that requires long-term monitoring. Responsibility for the environmental restoration and long-term monitoring was transferred from the DOE, National Nuclear Security Administration, Nevada Field Office to LM on October 1, 2006. The environmental restoration and site closure process were completed in 2015 in accordance with the Federal Facility Agreement and Consent Order (State of Nevada et al. 1996) (as amended) (FFACO) and all applicable Nevada Division of Environmental Protection (NDEP) policies and regulations. The Closure Report, Central Nevada Test Area, Subsurface Corrective Action, Unit 443 (LMS/CNT/S12760) (DOE 2016a) (Closure Report) describes LM’s plan for the long-term postclosure monitoring of radioisotope concentrations and water elevations, inspecting the site and maintaining the institutional controls (ICs), evaluating and reporting data, and documenting the site’s records and data management processes (DOE 2016a).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Spectral Induced Polarization-Biogeochemical Relationships for Remediation Amendment Monitoring

Geophysical tools such as electrical resistivity (ER) can indirectly monitor subsurface changes in response to remedial injections. These methods exhibit relatively low spatial resolution compared to sediment core characterization but are advantageous due to the ability to collect measurements non-intrusively over time across large volumes of the subsurface. Moreover, along with confirmatory groundwater or core sampling, geophysical methods can be used during active biogeochemical remedies to monitor short-term contaminant transformations and mobility, as well as part of an overall strategy for long-term monitoring of subsurface contaminated sites. The use of alternating current spectral induced polarization (SIP) provides significantly more information than conventional geophysical methods like direct current ER. SIP allows for monitoring changes in both solution and surface conductivity by separation of real and imaginary conductivity, respectively, as well as surface capacitance. In principle, SIP can measure indicators of remedy progression such as precipitation reactions that sequester contaminants, potentially providing a better indication of amendment delivery and reactivity as compared to conventional ER methods. However, multiple processes and material properties have overlapping (interacting) electrical responses across a range of frequencies. Hence, the purpose of this scoping study was to evaluate if SIP can be used to monitor (a) amendment delivery and (b) precipitation and reactivity of amendments under consideration at Hanford. SIP measurements were collected in fully saturated columns packed with sand and Hanford formation sediments containing (a) amendments that were highly conductive with significant capacitance (zero valent iron – ZVI, sulfur modified iron – SMI) and (b) amendments that exhibited low electrical conductivity with a small capacitance (calcite, apatite, bismuth). The sand was a quartz material with homogenous particle size that exhibited a relatively low surface conductivity. It was used as a control for comparison with the sediments from the Hanford Site, which have a greater surface conductivity because of their complex mineralogy and heterogeneous particle size distribution and may have complex interactions with amendments. The amendment mass fraction was varied to represent the different stages and subsurface locations associated with the delivery of a remedy. The primary objective was to identify the solution and solid surface changes associated with the delivery amendments and their secondary reactions within the subsurface. The figure below summarizes results for the amendments tested through this project. The SIP phase shift or imaginary conductivity change for the high conductivity amendments was more than 10 times that of the low conductivity amendments, highlighting the relative ease of detection of ZVI and SMI independent of the background signal from sand or Hanford sediments. The ZVI phase shift and imaginary conductivity changes occur primarily at high frequency (> 100 Hz) whereas SMI changes were at low frequency (0.01 to 10 Hz). SIP signals of SMI also increased over time and the maximum shifted to lower frequencies. The low conductivity amendments (calcite, abiotic and biotic apatite, bismuth subnitrate) exhibited relatively small phase and imaginary conductivity changes when added to sediments. The changes were above minimum detection limits (0.5 mrad for phase shift, 0.03 µS/cm for imaginary conductivity) for the highest concentration except for the commercial bismuth material. The lowest amendment concentration that can be detected is likely sediment specific, as minerals in sediments (clays, magnetite, Fe-oxides) have some capacitance and, therefore, exhibit a variable phase shift.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Detection of Organohalide-Respiring Enzyme Biomarkers at a Bioaugmented TCE-Contaminated Field Site

RNA-based biomarkers have been successfully detected at field sites undergoing in situ bioremediation, but the detection of expressed enzymes is a more direct way to prove activity for a particular biocatalytic process of interest since they provide evidence of potential in situ activity rather than simply confirming presence and abundance of genes in a given population by measurement of DNA copies using qPCR. Here we successfully applied shotgun proteomics to field samples from a trichloroethene (TCE)-contaminated industrial site in southern Ontario, Canada that had been bioaugmented with the commercially available KB-1 TM microbial culture. The KB-1 TM culture contains multiple strains of Dehalococcoides mccartyi (D. mccartyi) as well as an organohalide respiring Geobacter species. The relative abundances of specific enzymatic proteins were subsequently compared to corresponding qPCR-derived levels of DNA and RNA biomarkers in the same samples. Samples were obtained from two wells with high hydraulic connectivity to the KB-1 TM -bioaugemented enhanced in situ bioremediation system, and two control wells that showed evidence of low levels of native organohalide respiring bacteria (OHRB), Dehalococcoides and Geobacter . Enzymes involved in organohalide respiration were detected in the metaproteomes of all four field samples, as were chaperonins of D. mccartyi , chemotaxis proteins, and ATPases. The most highly expressed RDase in the bioaugmentation culture (VcrA) was the most highly detected enzyme overall in the bioaugmented groundwater samples. In one background groundwater well, we found high expression of the Geobacter pceA RDase. The DNA and RNA biomarkers detected using qPCR-based assays were a set of orthologs of Dehalococcoides reductive dehalogenases (VcrA, TceA, BvcA, dehalogenase “DET1545”), and the Ni-Fe uptake hydrogenase, HupL. Within a sample, RNA levels for key enzymes correlated with relative protein abundance. These results indicate that laboratory observations of TCE-bioremediation biomarker protein expression are recapitulated in field environmental systems and that both RNA and protein biomarker monitoring hold promise for activity monitoring of in situ populations of OHRB.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Promise of nonthermal plasmas in addressing emerging environmental and health problems: Present and future

Nonthermal atmospheric pressure plasmas transform input electrical energy efficiently into reactive species, charged particles, and photons. This “activated gas” is being investigated as solutions for a range of environmental and health problems facing society today. In this Perspective, we take a cursory look at a few of these societal problems and the reflected role that plasmas may play in charting the pathway to a solution buoyed by supporting research. Here, we survey the plasma-based opportunities in the removal of trace contaminants in water supporting methodologies such as water reuse, which addresses scarcity and pollution, the opportunity posed by plasmas-based chemical depolymerization for plastics recycling, and the application of plasmas for food security, which includes sterilization of foodstuffs and the improvement of crop yield. Finally, we also included a short review on how plasmas may help control disease spread. In each case, the scope of the problem is presented along with the potential plasma-based solution.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Ionic liquid mediated one-step perpendicular assembly in block copolymer thin films for ultrafiltration membrane applications

The rapid rise of oil and gas, petrochemical, food processing, and pharmaceutical industries has added a complex mixture of contaminants like oil, particulates, metals, and other organic compounds to wastewater. Multipurpose membranes with precise pore structure can offer a solution to this problem and block copolymers (BCP) can be used to achieve such structures. Achieving vertical assembly of BCP domains provides a perfect template for developing uniform through film channels for separation and transport of material, besides being useful for the rectification of defects in photolithography patterns. Producing such morphologies may require extensive film/substrate processing and is not always feasible for scale-up. With this article, we demonstrate a facile solution casting method to induce vertical domain assembly in as-cast diblock copolymer thin films in the presence of an ionic liquid (IL) additive that preferentially segregates to one block and neutralizes interfacial interactions. We also show the tunability of domain sizes by controlling the additive concentration. These vertically aligned morphologies are important for the development of next-generation lithographic techniques and form excellent templates for ultrafiltration membranes with uniform pore sizes. In conclusion, this article demonstrates how IL additives can be used to obtain stable non-equilibrium morphologies in as-cast BCP films and the effect of BCP molecular mass, block volume fractions, and IL content on self-assembly.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Inorganic Hydrogeochemistry in the 21st Century

Abstract Chemical and isotopic processes occur in every segment of the hydrological cycle. Hydrogeochemistry—the subdiscipline that studies these processes—has seen a transformation from “witch's brew” to credible science since 2000. Going forward, hydrogeochemical research and applications are critical to meeting urgent societal needs of climate change mitigation and clean energy, such as (1) removing CO 2 from the atmosphere and storing gigatons of CO 2 in soils and aquifers to achieve net‐zero emissions, (2) securing critical minerals in support of the transition from fossil fuels to renewable energies, and (3) protecting water resources by adapting to a warming climate. In the last two decades, we have seen extensive activity and progress in four research areas of hydrogeochemistry related to water‐rock interactions: arsenic contamination of groundwater; the use of isotopic and chemical tracers to quantify groundwater recharge and submarine groundwater discharge; the kinetics of chemical reactions and the mineral‐water interface's control of contaminant fate and transport; and the transformation of geochemical modeling from an expert‐only exercise to a widely accessible tool. In the future, embracing technological advances in machine learning, cyberinfrastructure, and isotope analytical tools will allow breakthrough research and expand the role of hydrogeochemistry in meeting society's needs for climate change mitigation and the transition from fossil fuels to renewable energies.

Zhu, Chen (ORCID:0000000153746787)↗
DOE OSTI2023

2020 Postclosure Groundwater Monitoring and Inspection Report, Central Nevada Test Area, Subsurface Corrective Action Unit 443

This report presents the groundwater monitoring data collected by the U.S. Department of Energy (DOE) Office of Legacy Management (LM) from the Central Nevada Test Area (CNTA), Nevada, Site, Subsurface Corrective Action Unit (CAU) 443 in Nye County, Nevada (Figure 1). The CNTA is the site of an underground nuclear test in 1968 that resulted in residual contamination near the detonation depth of 3200 feet (ft); the contamination requires long-term monitoring. Responsibility for the environmental restoration and long-term monitoring was transferred from DOE’s National Nuclear Security Administration, Nevada Field Office, to LM on October 1, 2006. The environmental restoration and site closure process were completed in 2015 in accordance with the amended 1996 Nevada Federal Facility Agreement and Consent Order (FFACO) (State of Nevada et al. 1996, as amended) and all applicable Nevada Division of Environmental Protection (NDEP) policies and regulations. The Closure Report, Central Nevada Test Area, Subsurface Corrective Action, Unit 443 (DOE 2018), also called the Closure Report, originally was completed in January 2016 and revised in October 2018; it describes LM’s plan for long-term postclosure monitoring. This includes monitoring of the radioisotopes of interest and water elevations, inspecting the site and maintaining the institutional controls (ICs), evaluating and reporting data, and documenting the site’s records and data management processes (DOE 2018).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

GIS-Based Modeling of Contaminated Soil Volumes at Multiple Sites in the Formerly Utilized Sites Remedial Action Program - 20149

The remediation of hazardous, toxic, and radioactive waste (HTRW) sites produces cost-related risks associated with the estimation of contaminated soil or debris volumes. Historical risk-management techniques include cost contingencies to cover volume uncertainties that affect project budgeting and decision-making. The Buffalo District teamed with project partners to lessen volume uncertainty and reduce project risks at multiple HTRW sites managed under the Formerly Utilized Sites Remedial Action Program (FUSRAP). Historical remedial investigations under FUSRAP commonly identified the presence of radiological material in site media, the associated human health risk, and then areas of remediation. To manage remedial execution and reduce risk, pre-design or remediation-phase sampling essentially 'chased' contamination, which was not conducive to efficient predictive budgeting derived from Feasibility Study (FS) cost analyses. The Buffalo District first optimized their approach to better understand volume uncertainty by utilizing the Argonne National Laboratory's Bayesian Approaches for Adaptive Spatial Sampling (BAASS) software [1]. BAASS processed soft data (e.g., gamma walk-over data) and spatial sampling data to estimate the lateral extent of contaminated soil irrespective of depth (i.e., gross contamination extent) and define areas of contaminant uncertainty. The software performed a binary transformation of contaminant concentrations at all sampling points based upon remedial action goals or a sum of ratios approach (i.e., clean, impacted, or range of impacts in soil). The model produced two-dimensional (horizontal) contaminant probability contours and statistical uncertainty in the sampling coverage and resulting contaminant extents. This method was translated vertically by partitioning the sampling data into depth brackets that produced a stacked representation of contaminant extents and uncertainty in the subsurface (i.e., similar to construction lifts). The results commonly led to a better understanding of project uncertainty and the need for sampling strategies that produce high-confidence soil volumes, which control costs. The BAASS-based delineations were eventually replaced by Empirical Bayesian Kriging (EBK) methods available in ArcGIS Spatial or 3D Analysts [2]. The EBK method calculates contaminant probability zones derived from user-controlled semivariograms of the spatial datasets. The resulting probability zones (e.g., 50% or 80% of contaminant probability) represent the two-dimensional surface delineation of the overall horizontal remedial area, similarly to BAASS. However, unlike BAASS, the vertical sampling data within these probability zones became vertical control points to contour a subterranean surface that connects subsurface points to the land-surface delineations of contamination. The resulting representation of horizontal and vertical impacts within an enclosed envelop (volume) of soil included uncertainty distributions that are used to plan uncertainty-reduction sampling. These data-driven and math-based models of three-dimensional sampling results produced well-bounded remedial volumes for project planning and better uncertainty predictions during project budgeting. The EBK method was applied to several FUSRAP sites managed by the Buffalo District and compared to less rigorously modeled sites previously remediated by the District. The comparison of modeled to actual remediated volumes provide a basis for validating the volume-estimation method. This comparison is important to ensure modeled volumes match physical boundaries of site remediation. FUSRAP sites with denser investigative sampling and lesser volume uncertainty proved useful in remedial planning and contracting. The Buffalo District noted that historical sites with sparser sampling arrays had greater disparity between estimated volumes and final remedial volumes. The benefit achieved over the cost of detailed soil sampling appears positive for FUSRAP projects, especially where impacts vary widely and appear unbounded by investigation-phase sampling. The subsequent Empirical Bayesian Kriging of contamination coupled with vertical contouring for soil estimations reduces uncertainty in soil volumes or indicates where sampling is required to reduce uncertainty, which together optimize remedial planning and budgeting. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Surface Processes Control the Fate of Reactive Oxidants Generated by Electrochemical Activation of Hydrogen Peroxide on Stainless-Steel Electrodes

Low-cost stainless-steel electrodes can activate hydrogen peroxide (H 2 O 2 ) by converting it into a hydroxyl radical ( • OH) and other reactive oxidants. At an applied potential of +0.020 V, the stainless-steel electrode produced • OH with a yield that was over an order of magnitude higher than that reported for other systems that employ iron oxides as catalysts under circumneutral pH conditions. Decreasing the applied potential at pH 8 and 9 enhanced the rate of H 2 O 2 loss by shifting the process to a reaction mechanism that resulted in the formation of an Fe(IV) species. Significant metal leaching was only observed under acidic pH conditions (i.e., at pH <6), with the release of dissolved Fe and Cr occurring as the thickness of the passivation layer decreased. Despite the relatively high yield of • OH production under circumneutral pH conditions, most of the oxidants were scavenged by the electrode surface when contaminant concentrations comparable to those expected in drinking water sources were tested. The stainless-steel electrode efficiently removed trace organic contaminants from an authentic surface water sample without contaminating the water with Fe and Cr. With further development, stainless-steel electrodes could provide a cost-effective alternative to other H 2 O 2 activation processes, such as those by ultraviolet light.

42 ENGINEERING↗
DOE OSTI2022

UV/chlorine advanced oxidation processes for degradation of contaminants in water and wastewater: A comprehensive review

Advanced oxidation processes (AOPs) have recently gained increasing attention as promising alternatives to conventional water and wastewater treatment technologies. As an AOP, there has been a growing interest in UV/chlorine due to its multiple disinfection modes and ability to maintain chlorine residuals in drinking water distribution systems. Compared to the popular UV/H 2 O 2 AOP treatment process, UV/chlorine AOP possesses several advantages including a higher radical production efficiency and a lower power demand. The process has recently been applied for the degradation of a wide range of natural and synthetic organic as well as inorganic compounds including pharmaceutical and personal care products, natural organic matter, herbicides and insecticides, taste and odor, and different types of water and wastewaters. The focus of the present work is to review and evaluate the efficiency of the UV/chlorine process on the oxidation of these pollutants. Here a critical overview is provided of the fundamentals of UV/chlorine, controlling factors of the process performance, and a comparison with other UV-based AOPs. The formation of disinfection by-products (DBPs), one of the concerns associated with UV/chlorine treatment, is discussed and strategies to tackle this obstacle are provided for future studies and applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Hydrogeological and hydrochemical investigation of groundwater using environmental isotopes ({sup 18}O, {sup 2}H, {sup 3}H, {sup 14}C) and chemical tracers: a case study of the intermediate aquifer, Sfax, southeastern Tunisia

Major element concentrations and stable (δ{sup 18}O and δ{sup 2}H) and radiogenic ({sup 3}H and {sup 14}C) isotopes in groundwater have proved useful tracers for understanding the geochemical processes that control groundwater mineralization and for identifying recharge sources in the semi-arid region of Sfax (southeastern Tunisia). Major-ion chemical data indicate that the origins of the salinity in the groundwater are the water–rock interactions, mainly the dissolution of evaporitic minerals, as well as the cation exchange with clay minerals. The δ{sup 18}O and δ{sup 2}H relationships suggest variations in groundwater recharge mechanisms. Strong evaporation during recharge with limited rapid water infiltration is evident in the groundwater of the intermediate aquifer. The mixing with old groundwater in some areas explains the low stable isotope values of some groundwater samples. Groundwaters from the intermediate aquifer are classified into two main water types: Ca-Na-SO{sub 4} and Ca-Na-Cl-SO{sub 4}. The high nitrate concentrations suggest an anthropogenic source of nitrogen contamination caused by intensive agricultural activities in the area. The stable isotopic signatures reveal three water groups: non-evaporated waters that indicate recharge by recent infiltrated water; evaporated waters that are characterized by relatively enriched δ{sup 18}O and δ{sup 2}H contents; and mixed groundwater (old/recent) or ancient groundwater, characterized by their depleted isotopic composition. Tritium data support the existence of recent limited recharge; however, other low tritium values are indicative of pre-nuclear recharge and/or mixing between pre-nuclear and contemporaneous recharge. The carbon-14 activities indicate that the groundwaters were mostly recharged under different climatic conditions during the cooler periods of the late Pleistocene and Holocene.

58 GEOSCIENCES↗
DOE OSTI2019

Consequence Analysis of Residual Water in a Storage Canister (Preliminary Report)

The objective of this work is to examine the consequences of a residual water on change in condition of cladding and SNF during dry storage. Small amounts of residual water may remain in SNF dry storage canisters after the fuel assemblies are transferred to the canister in the spent fuel pool (SFP), the canister is removed from the SFP and drained or pumped, vacuum dried in several pressure reducing steps, and backfilled with helium. This residual water from incomplete drying could degrade fuel rod cladding, oxidize exposed fuel pellets, and cause cladding failure resulting in SNF fines’ release in canister cavity. If residual water content is high enough, it could corrode internal components inside the canister, e.g., fuel basket, and neutron absorber plates, but CNWRA work indicated that corrosion of the internal component is expected to be negligible even with 55 moles of residual water. Considering this, focus of this work to determine partitioning of residual water towards fuel and cladding oxidation. Residual water will decompose by radiolysis and create reactive oxygen species, which, at sufficient high temperatures will oxidize cladding, and UO 2 exposed by clad breaches. If a significant fraction of UO 2 in a fuel rod is oxidized to U 3 O 8 , swelling of the fuel pellets will rupture the cladding and release fuel particles, contaminating the inside of the canister and complicating retrieval of fuel assemblies, transport and ultimate disposal. The report describes an evaluation of the potential cladding and exposed SNF pellets due to residual water. An integrated quantitative approach was used to estimate the effects. The approach consisted of (i) the evolution of environmental conditions, i.e., temperature and radiation field, in the cask, (ii) the physicochemical processes that affect degradation of the materials within the cask, and (iii) the potential damage states that may result from these conditions and processes. The assessment considers the following set of cask environmental conditions: (i) the quantity of residual water after drying, (ii) internal temperature fields and their intensity decrease over time, and (iii) the strength of the internal radiation field. The quantity of residual water will affect the mass of cladding, SNF, and other components that are degraded by oxidation. Temperature controls the rate of the oxidation reactions, the phase composition of water, and, to a lesser extent, the rate at which water vapor is radiolyzed. The strength of the radiation field controls the radiolysis rate of residual water. These processes, i.e., time evolution of temperature fields and their effects on radiolysis of residual water, fuel and cladding oxidations, were modeled using the integrated approach.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Integrated hydrogeophysical modelling and data assimilation for geoelectrical leak detection

Time-lapse electrical resistivity tomography (ERT) measurements provide indirect observations of hydrological processes in the Earth's shallow subsurface at high spatial and temporal resolution. ERT has been used in the past decades to detect leaks and monitor the evolution of associated contaminant plumes. Specifically, inverted resistivity images allow visualization of the dynamic changes in the structure of the plume. However, existing methods do not allow the direct estimation of leak parameters (e.g. leak rate, location, etc.) and their uncertainties. We propose an ensemble-based data assimilation framework that evaluates proposed hydrological models against observed time-lapse ERT measurements without directly inverting for the resistivities. Each proposed hydrological model is run through the parallel coupled hydro-geophysical simulation code PFLOTRAN-E4D to obtain simulated ERT measurements. The ensemble of model proposals is then updated using an iterative ensemble smoother. In this paper, we demonstrate the proposed framework on synthetic and field ERT data from controlled tracer injection experiments. Our results show that the approach allows joint identification of contaminant source location, initial release time, and solute loading from the cross-borehole time-lapse ERT data, alongside with an assessment of uncertainties in these estimates. We demonstrate a reduction in site-wide uncertainty by comparing the prior and posterior plume mass discharges at a selected image plane. This framework is particularly attractive to sites that have previously undergone extensive geological investigation (e.g., nuclear sites). It is well suited to complement ERT imaging and we discuss practical issues in its application to field problems.

58 GEOSCIENCES↗
DOE OSTI2022

Image Analysis for Rapid Assessment and Quality-Based Sorting of Corn Stover

Imaging in the visible spectrum is a low-cost tool that can be readily deployed for in-field or over-belt monitoring of biomass quality for bio-refining operations. Rapid image analysis coupled with innovative preprocessing may reduce the impacts of feedstock variability through identification of contaminants or other material attributes to guide selective sorting and quality management. Image analysis was employed to evaluate the quality of corn stover in red-green-blue (RGB) chromatic space. This study used controlled, bench-scale imaging as a proof-of-concept for rapid quality assessment of corn stover based on variations in material attributes, including chemical and physical attributes, that relate to biological degradation and soil contamination. Additionally, logistic regression-based classification algorithms were used to develop a method for biomass screening as a function of biological degradation or soil contamination. This study demonstrated the use of image analysis to extract features from RGB color space to investigate variations in critical material attributes from chemical composition of corn stover. Fourier transform infrared (FT-IR) suggested a correlation between red band intensity and biological degradation, while detailed surface texture analysis was found to distinguish among variations in ash. These insights offer promise for development of a rapid screening tool that could be deployed by farmers for in-field assessment of biomass quality or biorefinery operators for in-line sorting and process optimization.

09 BIOMASS FUELS↗