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At least 451 records · Page 25
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Assessment of the Degradation Mechanisms of Cu Electrodes during the CO 2 Reduction Reaction

Catalyst degradation and product selectivity changes are two of the key challenges in the electrochemical reduction of CO 2 on copper electrodes. Yet, these aspects are often overlooked. Here, we combine in situ X-ray spectroscopy, in situ electron microscopy, and ex situ characterization techniques to follow the long-term evolution of the catalyst morphology, electronic structure, surface composition, activity, and product selectivity of Cu nanosized crystals during the CO 2 reduction reaction. We found no changes in the electronic structure of the electrode under cathodic potentiostatic control over time, nor was there any build-up of contaminants. In contrast, the electrode morphology is modified by prolonged CO 2 electroreduction, which transforms the initially faceted Cu particles into a rough/rounded structure. In conjunction with these morphological changes, the current increases and the selectivity changes from value-added hydrocarbons to less valuable side reaction products, i.e. , hydrogen and CO. Hence, our results suggest that the stabilization of a faceted Cu morphology is pivotal for ensuring optimal long-term performance in the selective reduction of CO 2 into hydrocarbons and oxygenated products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Biota Dose Assessment at LANL for 2011

Beginning with the Manhattan Project, the earliest work with radioactive material was located in what is now the center of Los Alamos townsite, and some of those materials were released into the environment or disposed of as waste. These radioactive materials have been extensively studied and assessed in many reports during the past 60 years. The assessments consider many activities relevant to dose assessment, such as adventurous children who burrow into and eat the soil, as well as the activities of pets and wildlife. Even for the most extreme scenarios, the doses are less than a few mrem per year, well below the DOE limit for the public, and four orders of magnitude below the DOE limit to terrestrial animals, which is 0.1 rad per day. Locations that pose even a very small risk to humans or pets are fenced, locked, and posted as controlled areas. However, it is recognized that biota such as plants, birds, mice, and worms live in these controlled areas. The DOE standard is intended to protect these biota. Contaminated sites in and near Los Alamos consist of areas known as solid waste management units (SWMU) and areas of concern (AoC) that have been identified and studied extensively in many reports. LA-UR-90-4300 lists these locations, and many subsequent reports provide extensive details and assessments. Between these areas, the levels of detectable radioactive materials are many orders of magnitude smaller. Because they are not a focus of concern, the areas outside of SWMUs and AoCs have not been as extensively studied or sampled. The highest concentrations of radioactive materials resulting from historic LANL operations are buried in material disposal areas (MDAs) such as MDA A, B, C, G, T, etc. Much of this material is sealed in containers that are not accessible to biota (McNaughton 2005). In some cases, it is buried below the reach of tree roots or burrowing animals, and in some cases it is encased or embedded in concrete. Of particular relevance to the present report, the hills to the west of LANL, where the Las Conchas fire burned, are not contaminated with LANL‐derived substances. The radioactivity in these hills consists of naturally occurring radioactive material (NORM) and global fallout.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Carbon Capture Pilot at Vicksburg Containerboard Mill (Final Technical Report)

This is the final technical report for the DOE-OCED project DE-CD0000051. The report provides the progress at the close of the project. The objective of the project is to design and build a large pilot plant for carbon dioxide (CO 2 ) capture from a pulp and paper (P&P) mill using RTI’s non-aqueous solvent (NAS) technology at a capacity of 120,000 t-CO 2 /year, with >90% CO 2 captured. The pilot plant will be used for testing and evaluating the NAS capture process using real flue gas from the P&P mill’s power boiler for a minimum of 1 year of parametric testing and a minimum of 2,000 hours of continuous long-term testing. The testing will provide data for process optimization and scale-up for the P&P industry, provide information on interaction of flue gas contaminants on solvent performance and degradation, and inform strategies for emission control. At the end of the project, the pilot plant will be managed by International Paper (IP), the host site owner, which will continue to capture CO 2 , sequester the captured CO 2 , and be eligible for the 45Q credit.

42 ENGINEERING↗
DOE OSTI2023

Molten Salt Sampling Techniques and Analytical Approaches

Recent global interest in pyroprocessing and molten salt reactors has brought salt sampling methods and techniques back to the forefront of nuclear safeguards concerns. Issues with uranium supplies have also encouraged various countries to pursue advanced nuclear fuel cycles. Tracking nuclear material in molten salt has proven to be a challenge and updating molten salt sampling will greatly help in this endeavor. Molten salt is problematic to sample due to salt stratification, lack of homogeneity, solids, and difficulty with hot cell adaptations. Various salt sampling techniques have been used since before the 1960s including surface, spoon/spatula, and bar solidification. Since then, new types of sampling techniques have been developed to improve sampling results. These include rod/dip, pipet, suction, filtered sampling along with devices such as the Valve Core Sampler and the Multi-Level Sampler. These different approaches are being analyzed and improved upon along with developing requirements for an improved salt sampling device. Work continues to develop salt samplers that are more robust, easier to segment, collect at a specific depth, can work with filters, and can collect fines. Sampling parameters are also being narrowed in terms of stirring, settling time, filtration, depth, etc. In the future, we hope to address deficiencies for process control and nuclear material accountancy control by determining the best way to collect samples that minimizes contaminants and is representative. A compilation of salt sampling approaches, analyses techniques, and an evaluation of findings will be presented.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Investigation of Radiological Contamination at Parks in the Gateway National Recreation Area - 20350

In 2005, the National Park Service was notified that elevated radiation levels were detected at Great Kills Park during a baseline radiological mapping effort conducted by the Counter Terrorism Bureau of the New York City Police Department and the United States Department of Energy. Great Kills Park is in the Staten Island Unit of the Gateway National Recreation Area. A records search determined that approximately 280 acres of the park was established over an area in which the New York City Department of Sanitation placed approximately 15.1 million cubic yards of waste fill from 1944 to 1948. Since 2005, a series of response actions and investigations were conducted on behalf of the National Park Service to mitigate risk to human health and the environment and to determine the nature of radiological contamination at Great Kills Park. The findings support that radiological contamination is related to certain components of waste fill, including incinerator residue from both on and offsite incinerators, coal ash from the historical use of coal-fired boilers for heating, and incidental radiological artifacts in the waste fill due to their historical use and subsequent disposal. A majority of the radiological artifacts were determined to contain radium-226 and included radioluminescent markers, radium impregnated switch board buttons, radium paint containers, and brachytherapy devices. The National Park Service has several other Parks in the Gateway National Recreation Area that were established in areas with a similar history to Great Kills Park, and overlie waste fill historically placed during landfilling operations, including Spring Creek Park and Dead Horse Bay. Over the last year, the National Park Service has performed additional radiological investigations at Great Kills Park as part of the ongoing Remedial Investigation under the Comprehensive Environmental Response, Compensation, and Liability Act. In addition, preliminary radiological investigations were performed at Spring Creek Park and Dead Horse Bay Park in the Jamaica Bay Unit of Gateway National Recreation Area. These investigation activities identified gamma radiation levels above the ambient level, several of which were attributable to radiological artifacts similar in nature to those recovered at Great Kills Park. Ongoing investigations at Parks in the Gateway National Recreation Area support an association between radiological contamination and historical landfilling practices that were common prior to the regulation and control of radioactive materials. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Innovative use of Cr(VI) plume depictions and pump-and-treat capture analysis to estimate risks of contaminant discharge to surface water at Hanford reactor areas - 15315

The Hanford Site nuclear reactor operations required large quantities of high-quality cooling water, which was treated with chemicals including sodium dichromate dihydrate for corrosion control. Cooling water leakage, as well as intentional discharge of cooling water to ground during upset conditions, produced extensive groundwater recharge mounds consisting largely of contaminated cooling water and resulted in wide distribution of hexavalent chromium (Cr[VI]) contamination in the unconfined aquifer. The 2013 Cr(VI) groundwater plumes in the 100 Areas cover approximately 6 km{sup 2} (1500 acres), primarily in the 100-HR-3 and 100-KR-4 groundwater operable units (OUs). The Columbia River is a groundwater discharge boundary; where the plumes are adjacent to the Columbia River there remains a potential to discharge Cr(VI) to the river at concentrations above water quality criteria. The pump-and-treat systems along the River Corridor are operating with two main goals: 1) protection of the Columbia River, and 2) recovery of contaminant mass. An evaluation of the effectiveness of the pump-and-treat systems was needed to determine if the Columbia River was protected from contamination, and also to determine where additional system modifications may be needed. In response to this need, a technique for assessing the river protection was developed which takes into consideration seasonal migration of the plume and hydraulic performance of the operating well fields. Groundwater contaminant plume maps are generated across the Hanford Site on an annual basis. The assessment technique overlays the annual plume and the capture efficiency maps for the various pump and treat systems. The river protection analysis technique was prepared for use at the Hanford site and is described in detail in M.J. Tonkin, 2013. Interpolated capture frequency maps, based on mapping dynamic water level observed in observation wells and derived water levels in the vicinity of extraction and injection wells, are developed initially. Second, simulated capture frequency maps are developed, based on transport modelling results. Both interpolated and simulated capture frequency maps are based on operation of the systems over a full year. These two capture maps are then overlaid on the plume distribution maps for inspection of the relative orientation of the contaminant plumes with the capture frequency. To quantify the relative degree of protection of the river from discharges of Cr(VI) (and conversely, the degree of threat) at any particular location, a systematic method of evaluating and mapping the plume/capture relationship was developed. By comparing the spatial relationship between contaminant plumes and hydraulic capture frequency, an index of relative protectiveness is developed and the results posted on the combined plume/capture plan view map. Areas exhibiting lesser degrees of river protection are identified for remedial process optimization actions to control plumes and prevent continuing discharge of Cr(VI) to the river. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Integrated Modeling and Monitoring Technologies for Environmental Resiliency in Nuclear Energy

Environmental concerns pose the biggest challenge for the development of the nuclear energy industry, often preventing or limiting the construction of new plants and radioactive waste disposal facilities. There are currently numerous sites in the world at which surface and groundwater are contaminated by nuclear weapon production and testing, as well as due to nuclear power plant accidents. Many of those sites remain unused or inhabited primarily due to public concern. Improving scientific and technical capabilities to develop environmental resiliency is critical not only to address existing contamination, but also to build public confidence and support for nuclear energy. One of the obstacles in remediation is to tackle a large volume of contaminated soil and groundwater with relatively low concentrations. Although many contaminant removal technologies have developed (e.g., pump-and-treat systems), they are often expensive and not cost-effective for low-concentration radionuclide contamination. Although soil removal is often the most effective, it produces a large amount of waste that has to be stored securely for a long period of time or treated at the special treatment facilities. Transporting a large amount of waste may also produce greenhouse gases and disrupt local communities. Recently, the concept of 'sustainable remediation' has been proposed to improve a remediation system as a whole, including the consideration of cost effectiveness, reduction of greenhouse emission, waste production and energy usage. Rather than just focusing on removing contaminants, the sustainable remediation highlights the use of passive remediation technologies to immobilize radionuclides along with the application of monitored natural attenuation and longer institutional control. However, such passive technologies and monitored natural attenuation require the increased burden of proof to ensure that those immobilized contaminants would not compromise the long-term public health. Although contaminant transport modeling and risk assessments are always performed, they sometimes fail due to the lack of understanding the contaminant transport proposes at the time of the risk assessment or due to some unexpected processes. Monitoring technologies are critical to ensure the long-term stability of such remediated sites, and also to address the public concerns. Recent advances in in situ sensor technologies and spatially-extensive mapping technologies (such as unmanned aerial vehicles, airborne mapping, geophysics) have improved monitoring of contamination over space and time. In addition to new sensing devices, data management and data analytics technologies have been expanded to manage and process large spatial and temporal datasets. Such technologies can be used to reduce monitoring cost significantly, and to facilitate long-term monitoring. In this study, we demonstrate our data analytics technologies for two nuclear-related contaminated sites: (1) air dose rate monitoring in Fukushima prefecture, and (2) groundwater monitoring at the Savannah River Site F-Area. We are developing the spatial and temporal data integration methodologies to integrate various spatially extensive data and time-series data for improving long-term monitoring. Such monitoring technologies and experiences at the existing contaminated sites can be transferred to build a better monitoring system for nuclear facilities, such as nuclear power plants or nuclear waste storages.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Risk-Based Remediation Approach for Cs-137 Contaminated Sediment/Soils at the Savannah River Site (SRS) Lower Three Runs Tail (U) - 13348 - SRNS-RP-2012-00546

Lower Three Runs is a large blackwater stream that runs through the eastern and southern portion of the Savannah River Site. The Lower Three Runs watershed includes two SRS facility areas: P Area (P Reactor) and R Area (R Reactor) that provided effluent discharges to Lower Three Runs. During reactor operations, effluent discharges were well above natural (pre-industrial) or present day stream discharges. The watershed contains a 2,500-acre mainstream impoundment (PAR Pond), several smaller pre-cooler ponds, and a canal system that connects the pre-cooler ponds and discharges surface water to PAR Pond. From the PAR Pond dam, Lower Three Runs flows approximately 36 kilometers braiding through bottom-land/flood-plain forests before it enters the Savannah River. About eight kilometers downstream from the PAR Pond dam, the SRS boundary narrows (termed the Lower Three Runs tail) providing a limited buffer of DOE property for the Lower Three Runs stream and associated flood-plain. Previous screening characterization efforts revealed Cs-137 contamination in the sediment/soils of the flood-plain. As a part of the American Recovery and Reinvestment Act stimulus package, a comprehensive characterization effort was executed on the sediment/soils of the Lower Three Runs tail flood-plain providing a comprehensive look at the contaminant signature of the area. As a follow-up to that characterization, a regulatory decision Core Team, comprised of members of the South Carolina Department of Health and Environmental Control, Environmental Protection Agency - Region IV, and DOE, conducted negotiations on a risk-based approach to address the level of contamination found in the tail flood-plain as an early action that provided a long-term solution to exposure scenarios. For evaluation purposes, the adolescent trespasser was selected as the most likely human receptor for the Lower Three Runs tail portion because of the natural attractiveness of the area for recreational activities (i.e., hunting, fishing, hiking etc.) and access from public property. Exposure of the adolescent trespasser to Cs-137 contaminated sediment/soil at concentrations greater than 23.7 pico curies per gram have been calculated to result in an unacceptable cancer risk (> 1 x 10{sup -4}). Comparing the characterization sampling results conducted in 2009 with the benchmark concentration of 23.7 pCi/g, identified elevated risk levels along three sampling areas in the Lower Three Runs tail portion. On January 5, 2012, it was agreed by the core team that a Removal Action in the Lower Three Runs tail was to be conducted for the identified soil/sediment locations in the three identified areas that exceed the 1 x 10{sup -4} risk (23.7 pCi/g) for the adolescent trespasser receptor. The addition of Land Use Controls following the Removal Action was appropriate to protect human health and the environment. A systematic screening matrix was initiated at the identified hot spots (i.e., sampling points with Cs-137 activities greater than 23.7 pCi/g) to identify the limits of the excavation area. Sediment/soil within the defined removal areas would be excavated to the depth necessary to achieve the cleanup goal and disposed of in a CERCLA Off-Site Rule approved disposal facility. It was agreed that this removal action would adequately reduce the volume of available Cs-137 in the Lower Three Runs tail and consequently residual activities of the Cs-137 would decay over time reducing the amount of Cs-137 available in the tail which would curtail risk. The Land Use Controls consist of installation of an additional seven miles of fencing at major road crossings, utility easements, and at areas that showed a higher probability of access. In addition, signs were placed along the entire SRS perimeter of the Lower Three Runs tail approximately every 200 feet. Sign posts included both a No Trespassing sign and a Contaminant Warning sign. The project initiated a subcontract for both the removal action and the installation of fencing and signs on May 1, 2012. All field activities were completed by July 26, 2012. The project excavated and disposed of over 2700 cubic yards of contaminated sediment/soil, erected approximately seven miles of fence and placed over 2,000 signs demonstrating DOE's commitment to protect human health and act as a good neighbor to residents in the area. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

FX2 advanced fogging technology - 15711

Problem statement: The need for an advanced technology that can better address potential airborne contaminants at DOE Savannah River Site 235-F. Current methods of knocking down or fixing this contamination are labor intensive, costly, and sometimes ineffective. Thus, to make exposure ALARA, the advanced fogging effort is being tested using Idaho National Laboratory's FX2 fixative agent. The FX2 fogging agent is a proprietary mixture of water, latex paint (LTX), glycerin (GLY) and sodium lauryl sulfate (SLS). Initial development began in 2006 when a DOE Small Business Innovative Research (SBIR) grant resulted in the development of a conceptual advanced capture coating fog system. This coating is shown to be excellent at reducing airborne contamination and 'fixing' particulates in place as demonstrated by Idaho National Lab. Controlling Potential Airborne Particulates: Testing capacity to knockdown airborne particulates. Evaluating ability to fix to different surfaces (e.g., glass, wood, steel, concrete, brick). Line of sight as well as non-line of sight (shadowed) locations will be tested for coverage. Adhesiveness and Coverage of Surface Area: Contact area will be placed under air pressure to attempt dislodging of dried mixture. Particle analysis utilizing ImageJ will be conducted to determine quantifiable coverage. Ignitability: Observation of the FX2's reactivity to flame and heat sources as it is being applied. Results will provide useful information for the prevention of potential hazards. Determine Shielding Properties Against Alpha Sources: Determine the shielding abilities of the FX2. Fogging agent against an alpha particle emitting point source. Evaluating Critical Properties: These properties will be evaluated to better characterize the FX2 and allow for optimal understanding of results: ASTM E1354 - Burn Rate; NFPA 296-Flashover; ASTM D2196 - Viscosity; ASTM D1331 - Surface Tension; ASTM D792 - Density. Testing Innovations: Developed by the National Institutes of Health, ImageJ is a public domain image processing program that allows for the analysis that this effort requires. Coverage: Through contrast analysis, ImageJ can be used to determine the coverage of the agent upon any of the testing surfaces. Correlations: With the feature of coverage evaluation, a relationship, and thus a graphical representation, can be made between surface coverage and radiation shielding. Future work: Engineering and manufacturing of mobile robotic fogging device. ASTM WK5394: establishing performance specifications for stabilizers to minimize migration of dispersible radioactive contamination.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Innovative Use of Cr(VI) Plume Depictions and Pump-and-Treat Capture Analysis to Estimate Risks of Contaminant Discharge to Surface Water at Hanford Reactor Areas

The Hanford Site nuclear reactor operations required large quantities of high-quality cooling water, which was treated with chemicals including sodium dichromate dihydrate for corrosion control. Cooling water leakage, as well as intentional discharge of cooling water to ground during upset conditions, produced extensive groundwater recharge mounds consisting largely of contaminated cooling water and resulted in wide distribution of hexavalent chromium (Cr[VI]) contamination in the unconfined aquifer. The 2013 Cr(VI) groundwater plumes in the 100 Areas cover approximately 6 km2 (1500 acres), primarily in the 100-HR-3 and 100-KR-4 groundwater operable units (OUs). The Columbia River is a groundwater discharge boundary; where the plumes are adjacent to the Columbia River there remains a potential to discharge Cr(VI) to the river at concentrations above water quality criteria. The pump-and-treat systems along the River Corridor are operating with two main goals: 1) protection of the Columbia River, and 2) recovery of contaminant mass. An evaluation of the effectiveness of the pump-and-treat systems was needed to determine if the Columbia River was protected from contamination, and also to determine where additional system modifications may be needed. In response to this need, a technique for assessing the river protection was developed which takes into consideration seasonal migration of the plume and hydraulic performance of the operating well fields. Groundwater contaminant plume maps are generated across the Hanford Site on an annual basis. The assessment technique overlays the annual plume and the capture efficiency maps for the various pump and treat systems. The river protection analysis technique was prepared for use at the Hanford site and is described in detail in M.J. Tonkin, 2013. Interpolated capture frequency maps, based on mapping dynamic water level observed in observation wells and derived water levels in the vicinity of extraction and injection wells, are developed initially. Second, simulated capture frequency maps are developed, based on transport modelling results. Both interpolated and simulated capture frequency maps are based on operation of the systems over a full year. These two capture maps are then overlaid on the plume distribution maps for inspection of the relative orientation of the contaminant plumes with the capture frequency. To quantify the relative degree of protection of the river from discharges of Cr(VI) (and conversely, the degree of threat) at any particular location, a systematic method of evaluating and mapping the plume/capture relationship was developed. By comparing the spatial relationship between contaminant plumes and hydraulic capture frequency, an index of relative protectiveness is developed and the results posted on the combined plume/capture plan view map. Areas exhibiting lesser degrees of river protection are identified for remedial process optimization actions to control plumes and prevent continuing discharge of Cr(VI) to the river.

Miller, Chuck W.↗
DOE OSTI2019

Phosphate amendments for chemical immobilization of uranium in contaminated soil

Uranium (U) contamination is a major environmental problem associated with the mining and processing of nuclear materials for both weapons and power production. When possible, in situ soil remediation techniques are preferable for reducing the risk associated with diffuse low-level U contamination. Uranium is known to form sparingly soluble phosphate compounds that persist in the environment. Therefore, batch experiments were performed to evaluate the efficacy of three phosphate amendments, hydroxyapatite (HA), sodium phytate (IP6) and sodium tripolyphosphate (TPP), to immobilize U in contaminated sediments. The amendments were added at equivalent phosphorus (P) concentrations and then equilibrated under a range of test conditions, with changes in soluble U and Ptotal monitored at pre-set time intervals. Only HA was effective at reducing the soluble U soil fraction when compared to the control, with IP6 and TPP increasing the soluble U soil fraction. After equilibration, changes in contaminant partitioning in the amended sediments were evaluated using operational extraction methods. Sequential extraction results for HA generally indicated a transfer of U from labile to more recalcitrant phases, while the results for IP6 and TPP were more ambiguous.

Uranyl↗
DOE OSTI2022

Impacts of sulfonic acids on fungal manganese oxide production

Microbial manganese (Mn) oxidation plays a critical role in Mn(III/IV) oxide formation in modern day environmental systems. These oxidation processes and resulting biominerals are sensitive to aqueous conditions, such as pH and dissolved constituent concentrations. With Mn and sulfur (S) biogeochemical cycling closely linked in many environmental systems, and dissolved organic sulfur comprising a substantial pool of total sulfur in several environments, the impact of dissolved organic sulfur compounds on Mn redox processes is important to consider. Sulfonic acids, environmentally ubiquitous organosulfur compounds, play substantial roles in S cycling in many natural and contaminated systems. Research to assess the effects of these abundant sulfonic acids on Mn biogeochemical cycling, microbial Mn oxidation processes, and Mn biominerals is needed for understanding and predicting the impact of coupled S and Mn biogeochemical cycles, particularly in environments with dynamic redox gradients or in anthropogenically contaminated systems. Further, with research on microbial and abiotic Mn oxidation processes often using aminosulfonic acids to control pH, understanding the impact of such sulfonic acids on microbial Mn oxidation processes is critical. Several recent studies found that commonly used zwitterionic N substituted aminosulfonic acids, known as Good’s buffers, such as HEPES and MES, can alter abiotic birnessite sheet structures. Here we investigate the impact of two sulfonic acids with broad applications to natural and contaminated sites as well as laboratory settings (HEPES and MES) on fungal Mn oxidation relative to a carbonate buffer and a buffer-free control by three Ascomycete fungi known to oxidize Mn(II): Stagonospora sp. SRC1lsM3a, Paraphaeosphaeria sporulosa AP3s5–JAC2a, and Plectosphaerella cucumerina DS2psM2a2. Structural analyses of the products show that sulfonic acids promote Mn oxidation by P. cucumerina, producing hexagonally symmetric phyllomanganates analogous to hexagonal birnessite or c–disordered H + birnessite [(Ca,Na,K)(Mn 4+ ,Mn 3+ ,$\square$)O 2 nH 2 O], with solid–associated Mn(II) bound to vacancy sites and biomass, while in their absence almost all Mn remains as either aqueous Mn(II) or solid–associated Mn(II) bound to biomass. In contrast, sulfonic acids exert the opposite effect on Mn oxidation by P. sporulosa, with their presence suppressing Mn(II) oxidation to Mn(IV), likely leading to the formation of mycogenic bixbyite (Mn 3+ 2 O 3 ) while the buffer–free control forms a poorly crystalline phyllo- or tectomanganate. Meanwhile, all treatments exert a minimal effect on Mn(II) uptake from solution and Mn oxidation with Stagonospora sp., with all experimental systems and controls forming poorly crystalline, hexagonally symmetric phyllomanganates. The fact that the sulfonic acids here studied exert similar effects on Mn oxidation, but substantially different effects for each fungus, suggests they affect Mn oxidation via mechanistically similar pathways that are likely dependent on interactions with fungal exudates (which vary from species to species) or specific fungal Mn oxidation processes. Interestingly, for all fungi, MES increases Mn(III) in the resulting biominerals, while the carbonate buffer consistently decreases Mn(III). Further, these results clearly demonstrate that sulfonic acids not only alter Mn oxide structures, as has been previously noted in abiotic studies, but can interfere with Mn oxidation reactions themselves, highlighting the incredible sensitivity of both Mn oxide structures and the Mn oxidation process to the aqueous environment.

58 GEOSCIENCES↗
DOE OSTI2019

Current Status of Decommissioning Plans and Chemical Decontamination of Metal Scraps in Chinshan NPP - 19304

The decommissioning of nuclear facilities has become a significantly attractive and worldwide topic due to the end of lifetime of many nuclear power plants within next coming years. In Taiwan, Chinshan nuclear power plant owned by the Taiwan Power Company will be the first candidate to be decommissioned according to the Nuclear Reactor Facilities Regulation Act. The Chinshan nuclear power plant located in New Taipei City has two units of 636 MWe boiling water reactors (BWRs) for the generation of 9 billion kWh of electricity per year. The date of cessation of operation of Unit No. 1 and Unit No. 2 will be December in 2018 and July in 2019, respectively. Based on the Regulations for the Review and Approval of Applications for a Decommissioning Permit of Nuclear Reactor Facilities, Taiwan Power Company have submitted a decommissioning plan of Chinshan nuclear power plant to the authority, Atomic Energy Council (AEC). After the review process, the decommissioning plan of Chinshan nuclear power plant has been permitted by AEC in 2017. Decontamination is generally utilized during the period of decommissioning of nuclear facility in order to minimize the radiation exposure of personnel and the cost of management of radioactive wastes. The successful decontamination also probably provides the benefits of lowering the level of radioactive wastes, facilitating potential releases, permitting the reuse of metals and facilitating the radiation principle of As Low As Reasonably Achievable (ALARA) management. Decontamination aims at the removal of radioactive materials from the contaminated surfaces by several technologies such as washing, heating, chemical reaction and mechanical process. The selection of proper decontamination technologies are depended on the requirement of the target materials and the purpose of the decontamination. Chemical decontamination has been proven to be an effective in reducing the radioactivity for metallic materials by using chemical reagents in contact with the contaminated surfaces. During the operation of Chinshan nuclear power plant, chemical decontamination was performed for Unit No.1 and No.2 in 2000 to decontaminate the Reactor Recirculation System (RRS) and Reactor Water Clean-up Systems (RWCU) by using LOMI-NP-LOMI process. Based on the previous experience of chemical decontamination, the dismantled metallic piping is provided as sample by Chinshan nuclear power plant for the evaluation of the feasibility of chemical decontamination. The provided metallic sample is composed of carbon steel with dose rate around 0.2 mSv/hr. In this report, a multistep decontamination process using strongly oxidizing solution and organic acid solution is performed to remove the contaminated oxide layer from the metal surface, and the resulting contact dose rate and decontamination factor (DF) are also shown to discuss the performance in relation to the process control factors. In this paper, the recent progress in decommissioning programs and preliminary results of the decontamination experiment are described to provide usable information regarding the future decommissioning for Chinshan nuclear power plant. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Contribution of Microorganisms with the Clade II Nitrous Oxide Reductase to Suppression of Surface Emissions of Nitrous Oxide

The sources and sinks of nitrous oxide, as control emissions to the atmosphere, are generally poorly constrained for most environmental systems. Initial depth-resolved analysis of nitrous oxide flux from observation wells and the proximal surface within a nitrate contaminated aquifer system revealed high subsurface production but little escape from the surface. Further, to better understand the environmental controls of production and emission at this site, we used a combination of isotopic, geochemical, and molecular analyses to show that chemodenitrification and bacterial denitrification are major sources of nitrous oxide in this subsurface, where low DO, low pH, and high nitrate are correlated with significant nitrous oxide production. Depth-resolved metagenomes showed that consumption of nitrous oxide near the surface was correlated with an enrichment of Clade II nitrous oxide reducers, consistent with a growing appreciation of their importance in controlling release of nitrous oxide to the atmosphere. Our work also provides evidence for the reduction of nitrous oxide at a pH of 4, well below the generally accepted limit of pH 5.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Vivianite oxidation is not photocatalyzed

Vivianite is a hydrous Fe2+ phosphate mineral found in anoxic environments that plays an integral role in P cycling and environmental biogeochemistry. Imbued in the vivianite literature dating as far back as 1918 is the notion that vivianite is light-sensitive and susceptible to rapid photooxidation induced entirely by solar light. However, despite an exhaustive search, to our knowledge this conventionally accepted assumption has never been directly tested, nor has the band gap ever been measured. Resolving this question of photochemical control of vivianite redox chemistry is important for performing and interpreting experiments involving vivianite reactivity with contaminants, and potentially iron and phosphate cycling in the photic zone of aquatic systems. The present study was specifically designed to add¬ress this question. Pure synthetic vivianite samples were irradiated in aqueous suspensions with a Xe lamp at conditions mimicking the solar spectrum and compared to dark controls. Particles stirred in anoxic suspensions for up to 66 days showed no detectable oxidation irrespective of light exposure, according to colorimetric Fe2+/Fe3+ assays, micro X-ray diffraction, and Raman spectroscopy. In contrast, the same experiment performed using air-equilibrated suspensions showed systematic oxidation of up to ~80% mol% Fe(II) at 66 days, but again with no detectable light exposure effect. To test for UV reactivity, further experiments on vivianite powders under air versus N2 atmosphere were performed using a Hg lamp with a longpass filter. In contrast to oxidation in air where no effect of light was detected, after 24 hrs irradiation anoxically, 0.78% Fe was oxidized compared to dark controls, and after 13 days only an additional 0.3% Fe was oxidized. The band gap of pure vivianite was measured by the Tauc method to be 3.5 eV. Contrary to previous reports, solar light has minimal impact on the oxidation of pure vivianite, insignificant in particular when compared to its relatively fast oxidation by oxygen exposure. As such, light does not need to be excluded when running typical vivianite laboratory experiments. Long-term storage of natural vivianite in museums or private collections should continue protective measures given that a possible photocatalytic role of impurities cannot yet be ruled out. Nonetheless, at all depths in natural aquatic systems it appears that the primary abiotic control on the reactivity and half-life of vivianite particles should be the dissolved oxygen concentration, not light exposure.

Vivianite, photochemistry, oxidation↗
DOE OSTI2020

GaAs solar cells grown on intentionally contaminated GaAs substrates

III-V materials such as GaAs and GaInP have some of the best electronic and optical properties of any semiconductor materials, but deposition of these materials relies on high-quality single crystal GaAs substrates for their superior performance. Unfortunately, the cost of these substrates makes these high-efficiency devices only accessible in high-value or niche markets. In this study, we explore the effect of growing bulk GaAs crystals with lower purity input materials in order to reduce their cost. We observe that intentional impurities added to the melt before the crystal growth occurs segregate to the top of the boule. Single junction GaAs solar cells grown on substrates made from contaminated boules showed no performance degradation compared to a high-purity control substrate. These results suggest that lower purity Ga and As source materials can be used during crystal growth to reduce the cost of substrates.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Curvature-induced hydrophobicity at imogolite–water interfaces

Imogolite, a nanotubular aluminosilicate mineral, is commonly found in volcanic soils, where it exerts a control on carbon dynamics. Synthetic imogolites are used for the removal of contaminants from industrial effluents and are considered for a range of other applications including gas adsorption and functionalised heterogeneous catalysts. In spite of their environmental and industrial relevance, the properties of imogolite–water interfaces remain poorly understood. In this work, an experimental and computational study is presented in which the structure and energetics of water are characterized on the curved external surface of imogolite and the hydrophilicity of this surface is contrasted with that of gibbsite, its planar counterpart. Atomic force spectroscopy experiments show that in spite of their identical surface structure, imogolite has a lower hygroscopicity than gibbsite. Molecular dynamics simulations provide an explanation for this observation: the curvature of imogolite prevents the formation of in-plane H-bonds along the directions of the nanotube circumference, lowering the enthalpy of adsorption of water molecules. The different arrangement of surface H-bonds and the resulting differences in hydration properties also affects the acidity constants of surface hydroxyl groups. This ‘nanotube effect’ may be relevant to other nanotubular systems with high curvatures, potentially impacting their wetting properties, their colloidal stability and their affinity towards hydrophobic organic moieties.

36 MATERIALS SCIENCE↗