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Enhanced TcO 4 − reduction by metallic Fe 0 in the presence of particulate and structural Si. Rhythmical precipitation of dissolved iron leads to formation of layered structures related to geological phenomena such as orbicular rocks and Liesegang rings.
In the search for energy storage materials, metal octahydrotriborates, M(B3H8)n, n=1,2, are promising candidates but their synthesis suffers from residual solvents which tend to interact and greatly alter their decomposition mechanism. Therefore, we studied the thermal conversion of unsolvated Mg(B3H8)2 to BH4 -: as synthesized, and in the presence of MgH2. The conversion of our unsolvated Mg(B3H8)2 starts at ~100°C and yields ~22 wt% of BH4 - along with the formation of (closo-hydro)borates and volatile boranes. This loss of boron (B) is a sign of poor cyclability of the system. However, the addition of MgH2 to unsolvated Mg(B3H8)2 drastically increases the thermal conversion to 85-88wt% of BH4 - while simultaneously decreasing the amounts of B-losses. Our results strongly indicate that the presence of activated MgH2 substantially decreases the formation of (closohydro) borates and provides the necessary H2 for the B3H8-to-BH4 conversion. This is the first report of a metal octahydrotriborate system to selectively convert to BH4 - under moderate conditions of temperature (200°C) in less than 1h, making the MgB3H8-MgH2 system very promising for energy storage applications.
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Advanced instruments and methods need to be developed now to create a technical basis to support the negotiation of future nuclear arms control treaties. One new capability that is anticipated is the ability to confirm either the declared presence or declared absence of high explosive (HE) material in the presence of special nuclear material (SNM). Towards this goal, Passive HE Neutron Inspection (PHENIX) has been developed and demonstrated as a method for confirming the presence or absence of HE in the presence of plutonium. The method exploits the inherent presence of neutrons associated with the decay of plutonium as an internal probe source for performing prompt gamma-ray neutron activation analysis (PGNAA), searching for the presence of HE as revealed by the emission of characteristic gamma rays following neutron absorption in hydrogen and nitrogen which are building blocks of present-day, military-grade HE. Tests using stoichiometrically-correct hemishells of mock HE with plutonium show that a system can be expected to positively confirm the presence or absence of these signatures, supporting determination of HE presence or absence with Pu, in a few hours. To protect other potentially sensitive gamma-ray signatures from a treaty accountable item, an analog information barrier has been conceptualized and tested which physically prevents the collection of gamma-ray spectral data outside of user selected energy windows strategically chosen to view only narrow spectral regions corresponding to the hydrogen (2223.2 keV) and nitrogen (9807.2 keV, 10,318.2 keV, and 10,829.2 keV) PGNAA signatures.
Human settlements have historically thrived near rivers due to enhanced navigation and trade, and the availability of water supply and resources. The use of night light data, representing economic activities, provides a novel approach to studying the interactions between human activity and rivers over time. Here, we use the Defense Meteorological Satellite Program (DMSP) stable night light data from 2000 to 2013 as a proxy for human presence and activities to quantify the statistical relationships between night light presence and intensity in the Indus Basin, Asia. We test how these data are affected by proximity to trunk channels and by channel type (single/multi-thread) in the study area. We find that night light presence is enhanced by 26% within a 0 to 5 km proximity range of the Indus River and its tributaries, relative to the basin as a whole. We interpret this to represent increased human presence and activity within this zone. However, the mean intensity is lower near the river and higher away from the river, signifying denser settlements, such as towns and cities, which are preferentially located away from the Indus and its tributaries. Moreover, the enhancement of lit pixels signifying human presence and activities is increased by 18% near single-thread sections of the Indus River, compared to segments of the Indus displaying multi-thread morphologies. We suggest that this is due to the enhanced stability of single-threaded channels, relative to mobile multi-threaded channel reaches. This study demonstrates how night lights are an important tool in studying the relationship between human presence and river dynamics in large catchments such as the Indus, and we suggest that these data will have an important role in assessing differential flood spatial and social vulnerability at a regional scale.
Adsorption of noble gas fission products onto naturally occurring minerals is of interest for its potential to retain or retard emissions from nuclear fuel reprocessing operations or underground nuclear explosions. However, experimental studies of trace noble gas adsorption in the presence of air and water have largely focused on synthetic materials, such as activated carbon or metal-organic frameworks. Here, in this study, adsorption of Kr and Xe onto the naturally occurring zeolitic mineral clinoptilolite is studied in the presence of nitrogen and water. By varying the composition of the gas phase and monitoring the change in the combined adsorbate mass, the adsorbed concentration of noble gas is calculated gravimetrically. For dry clinoptilolite, the concentration of adsorbed Kr and Xe is linearly correlated with noble gas pressure and Henry's Law appears satisfactory, despite the presence of nitrogen at atmospheric pressures. However, the presence of water significantly reduces the adsorbed concentration of both Kr and Xe, which is typical in nanoporous sorbents. Here, an empirical bivariate model is presented, combining the Henry's Law adsorption model for a dry adsorbent with the exponential reduction in the presence of water, as reported by Lungu and Underhill in 1999. This model provides a means to estimate the adsorbate concentration at the trace partial pressures and higher water contents relevant to field-scale modeling of fission gas transport through the vadose zone.
Using hybrid functional-based density functional theory calculations, we analyze the structure and kinetics of defects formed in two competing synthesis routes to prepare hydrogen-doped In 2 O 3 films, using a hydrogen and oxygen gas mixture vs synthesis in the presence of water vapor. For both of these synthesis routes, we find that H + is the dominant defect species: when the Fermi level is close to the conduction band, H + has a lower formation energy than other intrinsic or extrinsic defects. Our results also suggest that water molecules spontaneously split into H + (which occupies octahedral voids) and OH – interstitials (which occupies vacant oxygen lattice sites or oxygen vacancies). From the analysis of the binding energies between these different defects, we conclude that these defects do not cluster and are most likely to stay spatially distributed throughout the films. In addition, the sum of formation energies of an oxygen (i.e., O$^{2–}_i$) and a H + interstitial is close to the formation energy of a OH – interstitial, meaning that water molecules are completely split into 2H + and O$^{2–}_i$ at the synthesis conditions. Further, in the presence of H 2 + O 2 gas mixture, oxygen interstitials occupy oxygen vacancies while hydrogen interstitials occupy vacant oxygen lattice sites and form bonds with lattice oxygens. Our analysis of the defect equilibria suggests that the hydrogen content in films synthesized in the presence of water vapor is higher than films synthesized in the presence of a hydrogen gas mixture. At high dopant concentrations, a hydrogen bond network is formed in the system and this leads to large distortions in the lattice.
Abstract Human impacts on the environment and wildlife populations are increasing globally, threatening thousands of species with extinction. While wildlife‐based tourism is beneficial for educating tourists, generating income for conservation efforts, and providing local employment, more information is needed to understand how this industry may impact wildlife. In this study, we used motion‐activated cameras at 12 waterholes on a private game reserve in northern Namibia to determine if the presence of humans and permanent infrastructure affected mammal visits by examining their (1) number of visits, (2) time spent, and (3) diel activity patterns. Our results revealed no differences in the number of visits based on human presence for any of the 17 mammal species studied. However, giraffes ( Giraffe camelopardalis ) spent more time at waterholes before observer presence compared to during. Additionally, several species changed diel activity patterns when human observers were present. Notably, several carnivore and ungulate species increased overlap in their activity patterns during periods while humans were present relative to when humans were absent. These modifications of mammal temporal activity patterns due to human presence could eventually lead to changes in community structure and trophic dynamics because of altered predator–prey interactions. As humans continue to expand into wildlife habitats, and wildlife‐based tourism increases globally, it is imperative that we fully understand the effects of anthropogenic pressures on mammal behavior. Monitoring of wildlife behavioral changes in response to human activity is crucial to further develop wildlife tourism opportunities in a way that optimizes the impact of conservation goals.
Grout materials are commonly used to immobilize low-level radioactive waste. Organic moieties can be unintentionally present in common ingredients used to make these grout waste forms, which may result in the formation of organo-radionuclide species. These species can positively or negatively affect the immobilization efficiency. However, the presence of organic carbon compounds is rarely considered in models or characterized chemically. Here, we quantify the organic pool of grout formulations with and without slag, as well as the individual dry ingredients used to make the grout samples (ordinary Portland cement (OPC), slag and fly ash), including total organic carbon (TOC) and black carbon, followed by aromaticity evaluation and molecular characterization via Electro Spray Ionization Fourier-Transform Ion Cyclotron Resonance Mass Spectrometry (ESI-FTICRMS). All dry grout ingredients contained significant amounts of organic carbon, ranging from 550 mg/kg to 6250 mg/kg for the TOC pool, with an averaged abundance of 2933 ± 2537 mg/kg, of which 60 ± 29% was composed of black carbon. The significant abundance of a black carbon pool implies the presence of the aromatic-like compounds, which was further identified by both phosphate buffer-assisted aromaticity evaluation (e.g., >1000 mg-C/kg as aromatic-like carbon in the OPC) and dichloromethane (DCM) extraction with ESIFTICRMS analysis. Besides aromatic-like compounds, other organic moieties were also detected in the OPC, such as carboxyl-containing aliphatic molecules. While the organic compound only consists of minor fractions of the grout materials investigated, our observations of the presence of various radionuclide-binding organic moieties suggests the potential formation of organo-radionuclides, such as radioiodine, which might be present at lower molar concentrations than TOC. Here, evaluating the role of organic carbon complexation in controlling the disposed radionuclides, especially for those radionuclides with strong association with organic carbon, has important implications for the long-term immobilization of radioactive waste in grout systems.
Results from experiments like LSND and MiniBooNE hint towards the possible presence of an extra eV scale sterile neutrino. The addition of such a neutrino will significantly impact the standard three flavor neutrino oscillations. In particular, it can give rise to additional degeneracies due to additional sterile parameters. For an eV scale sterile neutrino, the cosmological constraints dictate that the sterile state is heavier than the three active states. However, for lower masses of sterile neutrinos, the sterile state can be lighter than one and/or more of the three states. In such cases, the mass ordering of the sterile neutrinos also becomes unknown, along with the mass ordering of the active states. In this paper, we explore the mass ordering sensitivity in the presence of a sterile neutrino assuming the mass squared difference |Δ 41 | to be in the range 10 –4 –1 eV 2 . We study (i) how the ordering of the active states, i.e. the determination of the sign of Δ 31 gets affected by the presence of a sterile neutrino in the above mass range, (ii) the possible determination of the sign of Δ 41 for Δ 41 in the range 10 –4 –0.1 eV 2 . This analysis is done in the context of a liquid argon detector using beam neutrinos traveling a distance of 1300 km and atmospheric neutrinos that propagate through a distance ranging from 10 – 10000 km, allowing resonant matter effects. Apart from presenting separate results from these sources, we also do a combined study and probe the synergy between these two in giving an enhanced sensitivity.
Plutonium (Pu) redox and complexation processes in the presence of natural organic matter and associated iron can impact the fate and transport of Pu in the environment. In this work, we studied the fate of Pu(IV) in the presence of humic acid (HA) and Fe(II) upon reaction with H 2 O 2 that may be generated by photochemical and other reactions. A portion of Pu(IV) was oxidized to Pu(V/VI), which is primarily ascribed to the generation of reactive intermediates from the oxidation of Fe(II) and Fe(II)–HA complexes by H 2 O 2 . The kinetics of Pu(IV) oxidation is pH-dependent and can be described by a model that incorporates Pu redox kinetics with published HA-modified Fenton reaction kinetics. At pH 3.5, the presence of HA slowed Pu(IV) oxidation, while at pH 6, HA accelerated Pu(IV) oxidation in the first several hours followed by a reverse process where the oxidized Pu(V/VI) was reduced back to Pu(IV). Analysis of Pu-associated particle size suggests that Pu oxidation state is a major driver in its complexation with HA and formation of colloids and heteroaggregates. Our results revealed the H 2 O 2 -driven oxidation of Pu(IV)–HA–Fe(II) colloids with implications to the transient mobilization of Pu(V/VI) in organic-rich redox transition zones.
We explored the speciation and kinetics of the Pu(VI)-citrate and Pu(III)-citrate systems (pH m = 2.5–11.0, I = 0.1 M NaCl, T = 23 °C, O 2 (g) < 2 ppm) using ultraviolet–visible–near-infrared (UV–vis–NIR) spectrophotometry, solvent extraction, and PHREEQC modeling. Formation constants were determined for PuO 2 (HcitH)(aq) (log K° 1,1 = 1.09 ± 0.05) and PuO 2 (HcitH)(citH) 3– (log K° 1,2 = -0.20 ± 0.07), and evidence for (PuO 2 ) m (citH –k ) n (OH) x 2m(3+k)n–x was identified under alkaline conditions. Pu(VI) species were found to be less stable in the presence of citrate than in the absence of citrate (t ≤ 168 days); the rate of reduction increased with increasing pH. Further, the direct reduction of Pu(VI) to Pu(IV) was required to fit experimental data in the presence of citrate but did not improve the fit for Pu in the absence of citrate. We also observed increased Pu(III) stability in the presence of citrate (t ≤ 293 days), with higher concentrations of Pu(III) favored at lower pH. Finally, we provide evidence of a radiolysis-driven mechanism for the citrate-mediated reduction of plutonium that involves electron transfer from the oxidative breakdown of citrate. Our work highlights the need to investigate the redox effect of organic ligands on plutonium oxidation states under repository-relevant conditions.
Postconsumer polyolefins (r-POs) are leading plastic waste contributors today. This study reports, for the first time, the compatibilization of r-POs at a 50 kilogram (kg) scale with a styrene block copolymer compatibilizer in the presence of paraffin waxes as rheology modifiers (RMs). The addition of the rheological modifier (RM) and compatibilizer enhances the melt flow indices (MFIs) and mechanical properties, respectively. One aspect of this study is to compare the effectiveness of low-cost paraffin wax to that of specialized and expensive RMs in r-POs. The mechanical and rheological properties such as the melt flow index (MFI) of r-POs were compared in the presence of two types of RMs. Next, the study explores the challenges encountered when scaling the compatibilization of r-POs in the presence of paraffin wax from a 10-g to a 50-kg scale. The mechanical properties were determined and compared for samples at different scales. The study further investigated the effect of the method used for blending paraffin wax with r-PO and its impact on the value of their MFI and mechanical properties. This at-scale validation could pave the way for the commercialization of r-POs.
Borosilicate glasses are widely used for radioactive waste disposal due to their ability to incorporate a variety of contaminants and radionuclides while exhibiting high durability in various disposal scenarios. This research evaluated the dissolution of borosilicate glass using both single-pass-flow-through (ASTM C1662-18) and product consistency test (ASTM C1285-21) methods with different solutions, including a cementitious-contacted water (called grout-contacted, GC, from this point) and solutions with varying levels of dissolved cementitious species such as Si, Ca, Al. Here, the results indicated that the presence of Ca plays a crucial role in suppressing glass corrosion, as evidenced by the slower normalized dissolution rates, which were one order of magnitude lower for boron and two orders of magnitude lower for rhenium, observed in both Ca-amended and GC solutions compared to the pH 12 buffer solution. This effect is attributed to the formation of a dense, low-porosity, and strongly bonded calcium silicate hydrate (CSH) layer on the glass surface, which implies that a glass corrosion process is influenced by ion exchange involving alkali ions Na + , K + , Ca 2+ , and hydrogen-containing species. A small number of glass particles treated in the GC solution showed minor corrosion pits in the form of shallow craters with an average diameter of approximately 500 μm. This observation is correlated with a significant reduction, 2000 to 3000 times lower, in the cumulative volume of glass pores, indicating that smaller pore voids were “sealed” in the presence of Ca 2+ ions, likely attributed to the formation of CSH precipitation or other corrosion products such as calcium carbonate saturated from the grout solution. These findings suggest that the presence of dissolved Ca in the GC solution can slow down the dissolution of borosilicate glass, contrary to the expected trend of higher dissolution rates resulting from exposure to high alkaline and thus higher pH solutions.
Recent developments and tools integrated into the TAPaS code are presented, enabling realistic scenario simulations of particle dynamics within experimental tokamak magnetic equilibria. In particular, the enhanced capabilities of TAPaS enable seamless coupling with external simulations, provided the metric and equilibrium magnetic field of the external code are known. Coupling TAPaS with the gyro-fluid code FAR3d, the transport and losses of energetic particles in the presence Alfvén eigenmodes (AEs) in DIII-D plasma discharge #159243 were investigated. Detailed analyses of prompt losses with and without collisions were performed. Then, further analysis was performed in the presence of electromagnetic perturbations resulting from AEs activity. The results indicate that, for the energies and the initial conditions considered here, the presence of AEs enhances the particle losses.
In the United States, the true geographic distribution of the environmental fungus Histoplasma capsulatum remains poorly understood but appears to have changed since it was first characterized. Histoplasmosis is caused by inhalation of the fungus and can range in severity from asymptomatic to life-threatening. Due to limited public health surveillance and under detection of infections, it is challenging to directly use reported case data to characterize spatial risk. Using monthly and yearly county-level public health surveillance data and various environmental and socioeconomic characteristics, we use a spatio-temporal occupancy model to estimate latent, or unobserved, presence of H. capsulatum , accounting for imperfect detection of histoplasmosis cases. We estimate areas with higher probabilities of the presence of H. capsulatum in the East North Central states around the Great Lakes, reflecting a shift of the endemic region to the north from previous estimates. The presence of H. capsulatum was strongly associated with higher soil nitrogen levels. In this investigation, we were able to mitigate challenges related to reporting and illustrate a shift in the endemic region from historical estimates. This work aims to help inform future surveillance needs, clinical awareness, and testing decisions for histoplasmosis.
Here, an analysis is performed of how uncorrected antisymmetric aberrations, such as coma and trefoil, affect cryo-EM single-particle reconstruction (SPR) results, and an analytical formula quantifying information loss owing to their presence is inferred that explains why Fourier-shell coefficient-based statistics may report significantly overestimated resolution if these aberrations are not fully corrected. The analysis is validated with reference-based aberration refinement for two cryo-EM SPR data sets acquired with a 200 kV microscope in the presence of coma exceeding 40 µm, and 2.3 and 2.7 Å reconstructions for 144 and 173 kDa particles, respectively, were obtained. The results provide a description of an efficient approach for assessing information loss in cryo-EM SPR data acquired in the presence of higher order aberrations, and address inconsistent guidelines regarding the level of aberrations that is acceptable in cryo-EM SPR experiments.