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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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NASA NTRS2014

Humic Acid Complexation of Th, Hf and Zr in Ligand Competition Experiments: Metal Loading and Ph Effects

The mobility of metals in soils and subsurface aquifers is strongly affected by sorption and complexation with dissolved organic matter, oxyhydroxides, clay minerals, and inorganic ligands. Humic substances (HS) are organic macromolecules with functional groups that have a strong affinity for binding metals, such as actinides. Thorium, often studied as an analog for tetravalent actinides, has also been shown to strongly associate with dissolved and colloidal HS in natural waters. The effects of HS on the mobilization dynamics of actinides are of particular interest in risk assessment of nuclear waste repositories. Here, we present conditional equilibrium binding constants (Kc, MHA) of thorium, hafnium, and zirconium-humic acid complexes from ligand competition experiments using capillary electrophoresis coupled with ICP-MS (CE- ICP-MS). Equilibrium dialysis ligand exchange (EDLE) experiments using size exclusion via a 1000 Damembrane were also performed to validate the CE-ICP-MS analysis. Experiments were performed at pH 3.5-7 with solutions containing one tetravalent metal (Th, Hf, or Zr), Elliot soil humic acid (EHA) or Pahokee peat humic acid (PHA), and EDTA. CE-ICP-MS and EDLE experiments yielded nearly identical binding constants for the metal- humic acid complexes, indicating that both methods are appropriate for examining metal speciation at conditions lower than neutral pH. We find that tetravalent metals form strong complexes with humic acids, with Kc, MHA several orders of magnitude above REE-humic complexes. Experiments were conducted at a range of dissolved HA concentrations to examine the effect of [HA]/[Th] molar ratio on Kc, MHA. At low metal loading conditions (i.e. elevated [HA]/[Th] ratios) the ThHA binding constant reached values that were not affected by the relative abundance of humic acid and thorium. The importance of [HA]/[Th] molar ratios on constraining the equilibrium of MHA complexation is apparent when our estimated Kc, MHA values attained at very low metal loading conditions are compared to existing literature data. Overall, experimental data suggest that the tetravalent transition metal/-actinide-humic acid complexation is important over a wide range of pH values, including mildly acidic conditions, and thus, these complexes should be included in speciation models.

humic acid↗
NASA NTRS2011

More Surprises from the Moon

Even with the naked eye, the dark, extensive plains of the lunar maria can be clearly seen on the surface of the Moon. The maria formed after meteorite impacts created large craters that later filled with lava flows. Mare volcanism is the dominant type of volcanic activity on the Moon and the lavas are made up of basaltic rocks. However, non-mare volcanic deposits, though rare, have been observed on the lunar nearside. The deposits are distinguished from the maria because they are compositionally more evolved rich in silica, potassium and thorium. The deposits are limited in surface extent and it was unknown whether similar non-mare volcanism occurred at all on the Moon s farside. Writing in Nature Geoscience, Jolliff et al. report using Lunar Reconnaissance Orbiter images and compositional data to identify the rare occurrence of more compositionally evolved volcanic deposits in an isolated area on the Moon s farside. In the 1960s and 1970s, rock and soil samples were collected by the Apollo and Luna missions, by the USA and USSR respectively. This material represents a geologic treasure trove that continues to provide a wealth of information about the Moon and its evolution, and it was a very small fraction of these samples that gave the first hint that non-mare volcanic activity might have occurred. The samples contained fragments of complex volcanic rocks that were unrelated to the maria basalts. Violent bombardment of the Moon by meteorite impacts has caused significant mixing of the rocks at its surface, so the fragments could have had a source hundreds or thousands of kilometres away. The origin of the fragments was unknown. Several decades later, the Lunar Prospector mission used a gamma-ray spectrometer to map the distribution and abundance of various elements, including thorium, on the Moon s surface. The maps identified a distinct and large area of high thorium concentration, as well as several smaller, but equally peculiar areas of high thorium concentration on the nearside of the Moon (Fig. 1). The rocks that contained high thorium contents also exhibited geomorphological and spectral features that were typical of volcanic deposits, and so the thorium hotspots were thought to represent non-mare volcanism on the nearside of the Moon. A relatively large region with extremely high thorium concentrations - the Compton-Belkovich thorium anomaly - was also identified on the Moon s farside. This thorium hotspot was particularly unusual because it was completely isolated, alone on the farside of the Moon, far from the nearest maria. No high-resolution image data were available for this region, so a definitive interpretation of the source of this isolated anomaly has been impossible.

Petro, Noah↗
NASA NTRS1993

Th-230 - U-238 series disequilibrium of the Olkaria rhyolites Gregory Rift Valley, Kenya: Petrogenesis

Positive correlations of (U-238/Th-230) versus Th show the rhyolites to be products of partial melting. Positive correlations of U and Cl and U and F show that the U enrichment in the rhyolites is associated with the halogen contents which may be related to the minor phenocryst phase fractionation. Instantaneous Th/U ratios exceed time integrated Th/U ratios providing further evidence of the hydrous nature of the Olkaria rhyolite source. Excess (U-238/Th-230) in the subduction related rocks has been associated to the preferential incorporation of uranium in slab derived fluids, but no evaluation of the size of this flux has been made. The majority of the Naivasha samples show a (U-238/Th-230) less than 1 and plot close to the subduction related samples indicating the Naivasha rhyolites may also have been influenced by fluids during their formation. In general samples with high (U-238/Th-230) ratios reflecting recent enrichment of uranium relative to thorium have high thorium contents, thereby the high (U-238/Th-230) ratios are restricted to the most incompatible element enriched magmas and, hence, are a good indication that the rhyolites were formed by partial melting. If a fluid phase had some influence on the formation of the rhyolites then the uranium and thorium may have some correlation with F and Cl contents which can be mirrored by the peralkalinity. Plots of uranium against F and Cl contents are shown. The positive correlation indicates that the uranium enrichments are associated with the halogen contents. There seems to be a greater correlation for U against Cl than F indicating that the U may be transported preferentially as Cl complexes.

Black, S.↗
NASA NTRSDate not supplied

Mineralogical, Elemental, and Tomographic Reconnaissance Investigation for CLPS (METRIC): A Proposed Mission to the Lunar South Pole-Aitken Basin

The global Lunar Magma Ocean (LMO) hypothesis is based on analyses of ferroan anorthosites (FAN), magnesian plutonic rocks (Mg-suite), and KREEPy (Potassium - K; Rare Earth Elements - REE; Phosphorous - P) material present at the Apollo landing sites and the assumed global distribution of these lithologies. However, orbital spacecraft data over the last two decades have highlighted that the location of the Apollo missions within and near the Procellarum KREEP Terrane (PKT) is compositionally anomalous and not representative of the entire lunar surface and suggests that Apollo samples provide a biased view of the Moon. Further, meteorites, which originate from random areas on the lunar surface, including those not visited by Apollo, Luna, or Chang’E-5, provide complementary datasets that reveal a more complex lunar formation and evolution than the simple LMO onion skin model. While many recent investigations support and refine the LMO model, other recent studies have questioned whether this mechanism alone is responsible for the primordial differentiation of the Moon. Thus, relating the distinct and asymmetrically distributed geochemical terranes on the Moon, especially KREEP which is a predicted global LMO product, to lunar formation and differentiation remains a fundamental goal of lunar science. The South Pole-Aitken (SPA) impact carved a two-and-a-half thousand-kilometer basin into the Moon’s ancient crust, excavating material from as deep as the upper mantle. Orbital remote sensing of the basin indicates compositions with elevated thorium (Th) contents and unique mineralogies that provide a window into early lunar structure and LMO processes. We propose to land a powerful characterization laboratory at Birkeland crater on the far side of the Moon–where Th-rich SPA ejecta have been re-exposed near the surface–in order to address outstanding questions about the evolution of the Moon.

K M Cannon↗
NASA NTRS1999

Thorium Enrichment within the Procellarum KREEP Terrane: The Record in Surface Deposits and Significance for Thermal Evolution

The nearside-farside structural and compositional asymmetry of the Moon was recognized during the early days of Apollo and the suggestion was made that the migration of mantle melts to the nearside would have been favored by early Earth-Moon orbital dynamics and nonuniform planetesimal bombardment. Recent global geochemical mapping by Lunar Prospector has provided additional data, particularly in the Th distribution, that strongly supports the notion of global, preferential melt migration, which led in part to the development of the Procellarum KREEP Terrane (PKT) [2-5]. The surface distribution of Th was then reshaped by basin-forming impacts into the PKT, especially the Imbrium impact, which was the last and largest to strike in that region. The Imbrium event probably excavated material from a partially molten zone deep in the crust and delivered Th-rich ejecta Moon-wide. A fundamentally important but poorly understood aspect of the global Th distribution is the concentration of Th in the subsurface rocks of the PKT crustal section. For example, depending on what assumptions are made, the PKT crustal section, which is about 12% of the crust and only about 1.2% of the whole Moon, may contain as much as 40% of the Moon's entire Th budget. Such a distribution of Th and related heat-producing elements would have had a profound effect on melting, mixing, and the thermal evolution of the PKT and the underlying mantle. In this abstract, we examine the compositions of terra formations within the PKT and relate them to some of the Th-bearing rock types known from the Apollo samples. It appears that the existence of the PKT may be a unifying concept for a number of petrologic and geochemical observations. From the initial Lunar Prospector gamma-ray spectrometer data(-about 5 deg. resolution) and from the preliminary low-orbit data, there appears to be a number of relatively hotter "spots" within the PKT in terms of Th concentration. Some of the hotter spots correspond to intermediate-sized craters that penetrated volcanic flows and excavated Th-rich, submare material, such as Aristarchus, Aristillus, and Kepler. Other spots, however, correspond to surficial formations that constitute mainly rough topography associated with Imbrium ejecta or circum-Imbrium ring mountains and do not necessarily imply the presence of exposed KREEP basalts. The Fra Mauro Formation south of Copernicus toward the Apollo 14 site and regions of the Alpes Formation southwest of Copernicus in the vicinity of Reinhold lie within the most prominent hotspot; here them concentration is consistent with that found in the Apollo 14 soils (about 12-13 ppm) when the proportions of Fra Mauro Formation and mare basalt are considered. The area between Copernicus and Kepler and northwest of Copernicus in terra extending to the Carpathians is similarly enriched in Th. The Apennines from Eratosthenes toward the Apollo 15 site contain elevated Th concentrations, as does the northwestern quadrant of circum-Imbrium terra, especially between (but not including) La Condamine and Plato, and in the region northwest of the Jura mountains extending southward past Mairan to the Gruithuisen-Domes region. Within the main topographic rim of Imbrium, the Apennine Bench formation south of Archimedes appears to have relatively elevated Th concentration. Comparing the map of Th distribution to a digital-elevation map derived from Clementine altimetry, it appears that most of the areas richest in Th occur where the surface is elevated relative to the majority of PKT volcanic plains. Not all rough topography within the PKT has such elevated Th, however. Based on an analysis of the 5 deg. data, and using the calibration of, the mean Th concentrations for mainly volcanic-resurfaced terrain and rugged terrain are similar (about 5.5 ppm). This occurs in part because craters that penetrated mare basalt excavated Th-rich material. Even so, there appear to be extensive areas of volcanic resurfacing that have no obvious extrinsic source of Th-rich material, suggesting that the basalts, themselves, may contain as much as 5-6 ppm Th. High-FeO concentrations (18 to >20 wt%) indicate that these are not KREEP basalts but mare basalts. If so, this is surprising because most of the Apollo-sampled mare basalts have very low-Th (typically <2 ppm). A variety of Th-rich materials occur in the sample collection, particularly in the samples from the Apollo 12,14, and 15 sites. The most abundant Th-rich rock types are the mafic impact-melt breccias, which although found at all sites, are most abundant at Apollo 14, where they dominate the rock samples and make up some 40% of the rock particles in the soil. These have Th concentrations ranging up to about 30 ppm and averaging about 18 ppm. The Apollo 14 soils contain about 13 ppm Th, reflecting the high abundance of this melt-breccia component. At the nearby Apollo 12 site, the rocks consist mainly of mare basalts, and these have low-Th concentrations, mostly <1 ppm. Among the nonmare rocks, however, a few such as complex breccia 12013 contain a variety of evolved lithologies and represent potential sources of Th-rich components ranging from 17 to 50 ppm. A single fragment of KREEP basalt from the Apollo 12 soil contains about 50 ppm Th. Despite the identification of highly Th-enriched lithologic components at the Apollo 12 site, the soils there vary linearly in composition so as to extrapolate to a moderate Th KREEP-basalt component or a composition like that of the Fra Mauro formation as reflected by Apollo 14 soil (14 ppm Th at 10 wt% FeO). The nearby Lansberg Crater (39-km diameter) is a likely candidate to have delivered submare material such as buried Fra Mauro or Alpes material to the Apollo 12 site. Additional information contained in the original.

Jolliff, B. L.↗