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At least 793 records · Page 44
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Binding of uranyl cations to a Zr-based metal-organic framework by density functional theory

Zr-based metal–organic frameworks (Zr-MOFs) have been widely used as ion adsorbents for the removal or extraction of toxic and/or radionuclide species from aqueous solutions. However, the mechanisms by which uranyl cations (UO 2 2+ ) interact with Zr-MOFs have not been established. In this work, the nature of the bonding of uranyl cations with a Zr-MOF was determined using density functional theory for nineteen structurally distinct candidate complexes. Further, the results showed that in all cases the binding energy was of the order of 1.5 eV, but depended on the specific bonding site. The most stable structure involved coordination of the uranyl cation and two structurally distinct oxygens in the Zr-MOF metal node. It was also found that higher degree of deprotonation in Zr-MOF correlated with higher binding energy between the Zr-MOF and uranyl cations. These insights can aid in the design of Zr-MOFs with optimized features for efficient capture of uranyl cations.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Estimation of stress and stress-induced permeability change in a geological nuclear waste repository in a thermo-hydrologically coupled simulation

Geologic disposal is a promising solution for a safe permanent isolation of accumulated high-level nuclear waste from nuclear powerplants. The behavior of host rock is highly coupled thermally, hydromechanically, and chemically. Numerical simulations of such coupled phenomena for the extremely long term (>100,000 years) and large length scale (>1 km) of geologic disposal remain to be computationally challenging. In this study, a methodology has been developed to approximate stress and stress-induced permeability change in host rock using only thermo-hydrological (TH) variables. A coupled thermo-hydromechanical (THM) simulation is carried out using TOUGH-FLAC simulator to model THM behaviors of a generic nuclear waste repository, in order to evaluate the performance of the developed methodology, which is implemented in a coupled TH simulation. Results show that stress and permeability change estimated by the developed methodology in the TH-coupled simulation match those calculated in the THM-coupled simulation over the simulated timeframe of over 10,000 years. Details about errors in stress and permeability estimates accrued by the developed methodology are discussed here. The developed methodology will help incorporate stress-induced permeability change into existing TH simulators for the long-term radionuclide transport in geologic disposal.

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

Reduced-order modeling of near-field THMC coupled processes for nuclear waste repositories in shale

Performance assessment (PA) of geologic radioactive waste repositories requires three-dimensional simulation of highly nonlinear, thermo-hydro-mechanical-chemical (THMC), multiphase flow and transport processes across many kilometers and over tens to hundreds of thousands of years. Integrating the effects of a near-field geomechanical process (i.e. buffer swelling) into coupled THC simulations through reduced-order modeling, rather than through fully coupled geomechanics, can reduce the dimensionality of the problem and improve computational efficiency. In this study, PFLOTRAN simulations model a single waste package in a shale host rock repository, where re-saturation of a bentonite buffer causes the buffer to swell and exert stress on a highly fractured disturbed rock zone (DRZ). Three types of stress-dependent permeability functions (exponential, modified cubic, and Two-part Hooke’s law models) are implemented to describe mechanical characteristics of the system. Overall, our modeling study suggests that compressing fractures reduces DRZ permeability, which could influence the rate of radionuclide transport and exchange with corrosive species in host rock groundwater that could accelerate waste package degradation. Less permeable shale host rock delays buffer swelling, consequently retarding DRZ permeability reduction as well as chemical transport within the barrier system.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Public Health Response and Medical Management of Internal Contamination in Past Radiological or Nuclear Incidents: A Review

Following a radiological or nuclear emergency, workers, responders and the public may be internally contaminated with radionuclides. Screening, monitoring and assessing any internal contamination and providing necessary medical treatment, especially when a large number of individuals are involved, is challenging. Experience gained and lessons learned from the management of previous incidents would help to identify gaps in knowledge and capabilities on preparedness for and response to radiation emergencies. In this paper, eight largescale and five workplace radiological and nuclear incidents are reviewed cross 14 technical areas, under the broader topics of emergency preparedness, emergency response and recovery processes. The review findings suggest that 1) new strategies, algorithms and technologies are explored for rapid screening of large populations; 2) exposure assessment and dose estimation in emergency response and dose reconstruction in recovery process are supported by complementary sources of information, including ‘citizen science’; 3) surge capacity for monitoring and dose assessment is coordinated through national and international laboratory networks; 4) evidence-based guidelines for medical management and follow-up of internal contamination are urgently needed; 5) mechanisms for international and regional access to medical countermeasures are investigated and implemented; 6) long-term health and medical follow up programs are designed and justified; and 7) capabilities and capacity developed for emergency response are sustained through adequate resource allocation, routine nonemergency use of technical skills in regular exercises, training, and continuous improvement.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2020

Decontamination of urban surfaces contaminated with radioactive materials and consequent onsite recycling of the waste water

Enhancing rapid remediation strategies is paramount for recovery after a large-scale nuclear contamination event in an urban environment. Some current strategies recommend use of readily available equipment, materials, and facilities to expedite recovery. For example, applying pressurized water to contaminated surfaces may effectively remove radioactive contamination. In this study, a commercial power washer removes soluble forms of 152 Eu 3 + , 85 Sr 2 + , and 137 Cs + contamination from common porous building materials, and computer simulations characterize the recycling of the resultant contaminated wash water. Pressure washing the porous building materials under spray conditions typical with do-it-yourself units improved decontamination factors (DFs) for 152 Eu compared to low-pressure application of tap water (majority of two-tailed t-test p-values < 0.1), but pressure did not improve DFs for 137 Cs or 85 Sr. For both pressurized and low-pressure applications, adding potassium ions (K + ) to promote ion exchange reactions produced significantly higher DFs for tested radionuclides on asphalt, brick, and concrete. The resultant contaminated wash water can be processed through self-prepared chemical filtration beds of clay and sand. Modeled in a prior study, the beds yielded linear trends (R 2 > 0.98) in sensitivity analyses between most bed configuration variables and bed performance variables, permitting flexible ad-hoc bed design. The experimental and simulation results led to estimates of the remediation rate and waste generated after cleaning 250 m 2 of cesium-contaminated concrete from the combined deployment of a power washer and two different mobile treatment beds. Furthermore, the first treatment bed was designed to reduce treatment time and processed 1900 L of wash solution in 70 min using 880 kg of clay/sand infill material. Designed to reduce the solid waste generated, the second bed processed the same solution volume in 1040 min (17 h) using 170 kg of clay/sand infill material. The results of this analysis warrant further investigation of power washing with recycled salt solution as an effective rapid decontamination method with manageable waste.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

IUPAC-IUGS recommendation on the half-lives of 147 Sm and 146 Sm

In this paper, the IUPAC-IUGS joint Task Group “Isotopes in Geosciences” recommends a value of (106.25 ± 0.38) Ga for the half-life of 147 Sm, and a corresponding decay constant λ 147 = (6.524 ± 0.024) × 10 –12 a –1 , both with a coverage factor k = 2. For the extinct radionuclide 146 Sm two very different half-lives are used in the scientific community ( c . 68 and 103 Ma), to such a degree that no consensus value can be endorsed at present by the Task Group. Pending dedicated re-investigations it is recommended that papers using the 146 Sm decay to quantify the cosmo/geological evolution of (extra)terrestrial samples perform a twin set of calculations using both proposed half-lives.

146Sm↗
DOE OSTI2021

On the dissolution of a borosilicate glass with the use of isotopic tracing – Insights into the mechanism for the long-term dissolution rate

An understanding of the mechanisms responsible for controlling the long-term corrosion rate of nuclear waste glass is paramount if reliable glass dissolution models are to be used to calculate the controlled release of radionuclides from nuclear waste glass under geologic disposal conditions. Additionally, understanding silicate glass dissolution is also important for natural glasses to understand the role from the dissolution of these glasses has on the composition of natural aquatic systems. Two general mechanisms appear to be responsible for the elemental release from glass to the surrounding biosphere - ion exchange (release principally of alkalis) and matrix dissolution (release of the structural components of the glass). Key unknowns related to these mechanisms are the impact of surface layers on the altered glass and how these layers participate in corrosion. To better understand the impact of these layers on glass corrosion, we made two glasses of the same elemental composition, but with selected elements enriched in specific isotopes, e.g. more 10 B than 11 B. We reacted these glasses for 1 y then the solutions from each were exchanged and the chemistry of the solutions and the solids were followed for another 2 y and in some cases 3 y. This allowed us to follow changes in the glasses with respect to these elements and how these elements were transported through the alteration layers with time and, for at least one element, into the glass. Results from these experiments demonstrate that the release behavior of different elements is strongly dependent on their structural role in the glass (e.g. network formers and modifiers), but, more importantly, the role of water transport and subsequent ion exchange has in the long-term dissolution of the glass studied here. In this article, we highlight the behavior of four elements: lithium, sodium, silicon, and boron. Lithium and sodium, network modifying elements, have similar chemistries. The behavior of Li could be tracked in more detail by following both 6 Li and 7 Li; Li penetrates through the gel layer in both directions without hinderance and into and released from the glass deeper than sodium. Silicon, a network forming element, reacts with the silica-rich alteration layer. Boron, a network forming element, does not accumulate in the gel or the pristine glass and has a very sharp elemental profile between the pristine glass and alteration layer. Boron, lithium, and sodium elemental profiles suggest that there is little if any transport control within the alteration layer. The correlation between the Li and Na profiles and that of a water species suggest that the limiting release is a steady state between the diffusion of a water species and matrix dissolution that results in a low release rate for alkali and this provides a steady driving force for the long-term dissolution of glass.

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

Synthesis of results for Brine Availability Test in Salt (BATS) DECOVALEX-2023 Task E

In the 2023 phase of the international collaborative DECOVALEX modeling project, Task E focused on understanding thermal, hydrological, and mechanical (THM) processes related to predicting brine migration in the excavation damaged zone around a heated excavation in salt. Salt is attractive as a disposal medium for radioactive waste because it is self-healing and is essentially impermeable and non-porous in the far field. Investigation of the short-term, near-field behavior is important for radioactive waste disposal because this early period strongly controls the amount of inflowing brine. Brine leads to corrosion of waste forms and waste packages, and possible dissolution of radionuclides with brine transport being a potential transport vector to the accessible environment.The Task was divided into steps. Step 0 included matching unheated brine inflow data from boreholes at the Waste Isolation Pilot Plant (WIPP) and matching temperature observations during a Brine Availability Test in Salt (BATS) heater test. Step 1 included validation of models against a thermo-poroelastic analytical solution, and two-phase flow around an excavation. Finally, Step 2 required all the individual components covered in steps 0 and 1 to come together to match observed brine inflow behavior during the same BATS heater test.There were a range of approaches from the teams, from mechanistic to prescriptive. Given the uncertainties in the problem, some teams used one- or two-dimensional models of the processes, while other teams included more geometrical complexity in three-dimensional models. Task E was a learning experience for the teams involved, and feedback from the modeling teams has led to changes in follow-on BATS experiments at WIPP. The primary Task E lessons learned were the impact of hydrologic initialization methods (wetting up vs. drying down), the difference between confined and unconfined thermal expansion, and the large changes in permeability associated with heating and cooling.

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

Resilient design in nuclear energy: Critical lessons from a cross-disciplinary analysis of the Fukushima Dai-ichi nuclear accident

This paper presents a multidisciplinary analysis of the Fukushima Dai-ichi Nuclear Power Plant accident. Along with the latest observations and simulation studies, we synthesize the time-series and event progressions during the accident across multiple disciplines, including in-plant physics and engineering systems, operators’ actions, emergency responses, meteorology, radionuclide release and transport, land contamination, and health impacts. We identify three key factors that exacerbated the consequences of the accident: (1) the failure of Unit 2 containment venting, (2) the insufficient integration of radiation measurements and meteorology data in the evacuation strategy, and (3) the limited risk assessment and emergency preparedness. We conclude with new research and development directions to improve the resilience of nuclear energy systems and communities, including (1) meteorology-informed proactive venting, (2) machine learning-enabled adaptive evacuation zones, and (3) comprehensive risk-informed emergency planning while leveraging the experience from responses to other disasters.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
DOE OSTI2020

Evaluation of Gaseous Substrates for Microbial Immobilization of Contaminant Mixtures in Unsaturated Subsurface Sediments

Extensive vadose zone metals and organic contamination remains at many former industrial and defense manufacturing sites, and effective remedial solutions are needed to slow or prevent its migration to groundwater. In this study, the application of gaseous substrates to stimulate microbial respiratory reduction of comingled radioisotopes and nitrate under unsaturated conditions was examined for possible application at the Hanford Site, a former nuclear production facility in southeastern WA, USA. First, screening studies were performed to qualitatively measure the sediment respiratory response to 14 gaseous or volatile organic substrates at two moisture contents, 4% and 8%. Volatile substrates produced the strongest respiratory response, among them were butyrate, pentane, butyl acetate. Ethane and butane were the most effective gaseous substrates but only at 8% water content. Hanford sediment from two waste sites with distinctive chemistries were wetted to 7% moisture content, packed into columns, and treated with ethane or butane. After 4 weeks, columns were then leached to quantify retardation in the mobility of aqueous contaminant concentrations compared to no gas control columns. Treatment with both gases resulted in >80% removal of Cr from the aqueous phase. However, NO3 concentration and a waste sites exposure history to NO3 had a major effect on U and Tc reduction. Incomplete nitrate reduction outcompeted U and Tc in waste site sediments having limited prior exposure to NO3. Conversely, waste site sediments co-contaminated with NO3 were able to achieve highly reduced conditions resulting in complete denitrification of NO3, and delayed leaching of U and Tc. This implied effective reduction of both contaminants to less mobile species. This study demonstrates that unsaturated vadose sediments at Hanford waste sites have the capacity for a sustained respiratory response to gaseous substrate injection, which could potentially be deployed as part of an overall strategy to reduce the flux of long-lived radionuclides to groundwater at Hanford and other legacy waste sites.

Bagwell, Christopher E.↗
DOE OSTI2020

Optimal methods for preparation, separation, and determination of radium isotopes in environmental and biological samples

In recent years, radium has attracted considerable attention primarily because of the rapid increase in unconventional (fracking) drilling technology in the United States and around the world. One of the major radionuclides of interest in unconventional drilling wastes is radium isotopes ( 224 Ra, 226 Ra, 228 Ra). To access long-term risks associated with radium isotopes entering into the environment, accurate measurements of radium isotopes in environmental and biological samples are crucial. This article reviews many aspects of radium chemistry, which includes recent developments in radiochemical separations methods, advancements in analytical techniques followed by a more detailed discussion on the recent trends in radium determination.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Evaluation of several relevant fractionation processes as possible explanation for radioxenon isotopic activity ratios in samples taken near underground nuclear explosions in shafts and tunnels

Gas samples taken from two historic underground nuclear tests done in 1989 at the Nevada National Security Site (NNSS), formerly the Nevada Test Site (NTS), were examined to determine how xenon isotopes fractionate because of early-time cavity processes, transport through the rock, or dispersal through tunnels. Xenon isotopes are currently being used to distinguish civilian sources of xenon in the atmosphere from sources associated with underground nuclear explosions (UNEs). The two nuclear tests included (1) BARNWELL, a test conducted in a vertical shaft approximately 600 m below ground surface at Pahute Mesa, and (2) DISKO ELM, a horizontal line-of-sight test done in P-tunnel approximately 261 m below the surface of Aqueduct Mesa. Numerical flow and transport models developed for the two sites had mixed success when attempting to match the observed xenon isotope ratios. At the BARNWELL site, the simulated xenon isotope ratios were consistent with measurements from the chimney and ground surface and appeared to have been affected primarily by fractionation during subsurface transport. At the DISKO ELM site, samples taken from two elevations in the chimney failed to show the degree of fractionation predicted by the models during transport and did not show evidence for significant fractionation due to early-time condensation of refractory xenon-precursor radionuclides into the melt glass. Gas samples taken from the adjacent tunnels in the days following the test showed mixed evidence for early-time separation of xenon isotopes from their iodine precursors.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Iron-rich microstructure records of high temperature multi-component silicate melt behavior in nuclear fallout

Above-ground nuclear explosions that interact with the surface of the earth entrain materials from the surrounding environment, influencing the resulting physical and chemical evolution of the fireball, which can affect the final chemical phase and mobility of hazardous radionuclides that are dispersed in the environment as fallout particles. The interaction of iron with a nuclear explosion is of specific interest due to the potential for iron to act as a redox buffer and because of the likelihood of significant masses of metals to be present in urban environments. We investigated fallout from a historic surface interacting nuclear explosion conducted on a steel tower and report the discovery of widespread and diverse iron-rich micro-structures preserved within the samples, including crystalline dendrites and micron-scale iron-rich spheres with liquid immiscibility textures. We assert these micro-structures reflect local redox conditions and cooling rates and can inform interpretation of high temperature events, enabling new insights into fireball condensation physics and chemistry when metals from the local environment (i.e. structural steel) are vaporized or entrained. Finally, these observations also significantly expand the availability of silicate immiscibility datasets applicable to rapidly quenched systems such as meteorite impact melt glass.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Projected network performance for next generation aerosol monitoring systems

Aerosol monitoring for radioactivity is a mature and proven technology. However, by improving key specifications of aerosol monitoring equipment, more samples per day can be collected and analyzed with the same minimum detectable concentrations as current systems. This work models hypothetical releases of 140 Ba and 131 I over a range of magnitudes corresponding to the inventory produced from the fission of about 100 g to 1 kiloton TNT-equivalent of 235 U. The releases occur over an entire year to incorporate the natural variability in atmospheric transport. Sampling equipment located at the 79 locations for radionuclide stations identified in the Comprehensive Nuclear-Test-Ban Treaty (CTBT) for the International Monitoring System are used to determine the detections of the individual releases. Alternative collection schemes in next generation equipment that collect 2, 3, or 4 samples per day, rather than the current 1 sample per day, would result in detections in many more samples at more stations with detections for a given release level. The authors posit that next generation equipment will result in increased network resilience to outages and improved source-location capability for lower yield source releases. The application of dual-detector and coincidence measurements to these systems would significantly boost sensitivity for some isotopes and would further enhance the monitoring capability.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

Preferential adsorption of noble gases in zeolitic tuff with variable saturation: A modeling study of counter-intuitive diffusive-adsorptive behavior

Noble gas transport through geologic media has important applications in the prediction and characterization of measured gas signatures related to underground nuclear explosions (UNEs). Retarding processes such as adsorption can cause significant species fractionation of radionuclide gases, which has implications for measured and predicted signatures used to distinguish radioxenon originating from civilian nuclear facilities or from UNEs. Accounting for the effects of variable water saturation in geologic media on tracer transport is one of the most challenging aspects of modeling gas transport because there is no unifying relationship for the associated tortuosity changes between different rock types, and reactive transport processes such as adsorption that are affected by the presence of water likewise behave differently between gas species. In this study, we perform numerical diffusive-adsorptive transport simulations to estimate gas transport parameters associated with bench-scale laboratory diffusion cell experiments measuring breakthrough in zeolitic and non-zeolitic rocks for a gaseous mixture of xenon, krypton, and SF 6 at varying degrees of water saturation (S w ). Counter-intuitive transport behavior was observed in the zeolitic rock experiments whereby breakthrough concentrations were significantly higher when the core was partially saturated (S w = 17 %) than under dry (S w = 0 %) conditions. Breakthrough of xenon was especially retarded in the dry core – likely due to comparatively high affinity of xenon for zeolitic adsorption sites – and estimated effective diffusion coefficients for all gases were approximately an order of magnitude lower than what is predicted by porosity-tortuosity models. We propose the counter-intuitive behavior observed is because water infiltration of zeolite nanopores reduces both the adsorptive capacity of the rock and the tortuosity of connected flow paths. We developed a two-site competitive kinetic Langmuir adsorption reaction for the porous media transport simulator in order to constrain transport parameters within zeolitic tuff, where differential adsorption to zeolite and non-zeolite pores was observed. We determined that liquid saturation-dependent diffusive-adsorptive transport is affected by subtle and at times competing processes that are specific to different gases, which have a significant overall influence on effective transport parameters.

58 GEOSCIENCES↗
DOE OSTI2025

Uptake and elimination of 137Cs in aquatic biota inhabiting a contaminated effluent canal

Radiocesium (137Cs) is among the most prevalent and concerning radionuclide released from anthropogenic activities due to its relatively slow decay time and high bioavailability. Numerous studies have reported activity concentrations of 137Cs in exposed biota, but few have assessed detailed toxicokinetics. The objective of our study was to quantify and compare the uptake and elimination of 137Cs in aquatic taxa from multiple classes with different ecological roles inhabiting a canal contaminated from nuclear production activities on the Savannah River Site in South Carolina, USA. We tracked accumulation and elimination of 137Cs in four understudied aquatic species: one aquatic macrophyte [American white water lily (Nymphae odorata), two benthic associated omnivorous species (American bullfrog (Lithobates catesbeianus) and red swamp crayfish (Procambarus clarkii), and one pelagic carnivorous fish (Eastern mosquitofish (Gambusia holbrooki)]. We monitored accumulation of 137Cs from initial exposure until equilibrium for biota restricted within the canal and subsequently tracked elimination of 137Cs over time by moving organisms from the canal to a nearby reference pond. Results indicated bullfrog tadpoles reached 95 % equilibrium in approximately 9 days, the fastest among the species evaluated. After bullfrog tadpoles, the next fastest time to equilibrium was achieved by red swamp crayfish (51 days) followed by mosquitofish (86 days). At equilibrium, bullfrog tadpoles were found to have similar 137Cs activity concentrations to mosquitofish (3.16 and 3.57 Bq/g, respectively), and both were significantly higher than red swamp crayfish (1.77 Bq/g). For elimination, we found biological half-lives to range between 8 and 43 days with bullfrog tadpoles eliminating 137Cs the fastest followed by water lilies, mosquitofish, and red swamp crayfish. Overall, we found the uptake and elimination of 137Cs to vary widely among our studied species, but benthic organisms are not at an increased risk to accumulate 137Cs compared to organisms in less frequent contact with the sediment.

Benthic organism Bioaccumulation Bioindicator Elim↗
DOE OSTI2025

Analysis of measurements from an array of radioxenon samplers near to Hartlepool Nuclear Power Station

As part of a scientific research and development project, the radionuclide fingerprint of an operating advanced gas-cooled reactor 25 (AGR) has been studied across several facets (Goodwin et al., 2024). One part of this project was to deploy an array of 26 radioxenon samplers to the region for a period of around 1 year, to measure any radioxenon emissions from the reactors of the 27 Hartlepool nuclear power station at a range of tens of kilometres away. The array of 3 sensors was operational for around 12 28 months from March 2022 and detected many occurrences of isotopes of radioxenon. Here we provide a detailed analysis and 29 interpretation of the data and where possible, attribution of detections to a source or region. Whilst a key part of this work is to 30 measure any emissions of radioxenon from Hartlepool, this work presents one of the most comprehensive efforts to determine the 31 source of a great number of (mostly) 133Xe detections. A combination of different types of atmospheric dispersion modelling 32 techniques, including the use of stack monitoring data from nearby civil radioxenon-emitting nuclear facilities has enabled the 33 majority of detections to be attributed to one or more possible sources. Whilst emissions from Hartlepool have been detected on 34 the systems, the majority of detections are associated with a medical isotope production facility in Fleurus, Belgium (IRE).

Advanced gas-cooled reactor↗
DOE OSTI2021

Solid phase characterization and transformation of illite mineral with gas-phase ammonia treatment

In situ remediation applications of ammonia (NH 3 ) gas have potential for sequestration of subsurface contamination. Ammonia gas injections initially increase the pore water pH leading to mineral dissolution followed by formation of secondary precipitates as the pH is neutralized. However, there is a lack of understanding of fundamental alteration processes due to NH 3 treatment. In these batch studies, phyllosilicate minerals (illite and montmorillonite) were exposed to NH 3 gas with subsequent aeration to simulate in situ remediation. Following treatments, solids were characterized using a variety of techniques, including X-ray diffraction, N 2 adsorption-desorption analysis for surface area, Fourier transform infrared (FTIR) spectroscopy, nuclear magnetic resonance (NMR), and microscopy methods to investigate physicochemical transformations. The results of this study indicate that, at high pH, the clays are altered as observed by differences in morphology and particle size via microscopy. However, the two clays interact differently with NH 3 . While montmorillonite interlayers collapsed due to intercalation, illite layers were unaffected as confirmed by FTIR analysis. Further, structural changes in silicate ([SiO 4 ] n- ) and aluminol (Al-OH) groups were identified by NMR and FTIR. This research showed that mineral alteration processes occur during and after NH 3 gas treatment which may be used to remove radionuclides from the aqueous phase through sorption, co-precipitation, and coating with secondary phyllosilicate alteration products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗