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At least 631 records · Page 35
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Synthesis and structural characterization of a hydrated sodium–caesium tetracosatungstate(VI), Na 5 Cs 19 [W 24 O 84 ]·21H 2 O

Crystal formation of penta­sodium nona­deca­cesium tetra­cosa­tungstate(VI) heneikosahydrate, Na 5 Cs 19 [W 24 O 84 ]·21H 2 O, was successfully achieved by the conversion of [H 2 W 12 O 42 ] 10– through the addition of excess Cs + . The crystal structure comprising the toroidal isopolyoxidometalate is presented, as well as its Raman spectrum. Na 5 Cs 19 (H 2 O) 21 W 24 O 84 crystallizes in the rhombohedral space group R$\overline{3}$ with an obverse centering. The title compound represents the addition of a new member to the isopolytungstate family with mixed alkali counter-ions and contains rarely observed five-coordinate tungsten(VI) atoms in the [W 24 O 84 ] 24– anion (site symmetry C 3i ) arising from the conversion mediated by Cs + counter-ions.

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

Evaluation of Mechanical and Thermomechanical Water Vapor Compression Techniques for Enabling High Temperature Lift Hydration-Based Chemical Heat Pumps

Achieving high temperature lifts (>200 K) via a chemical heat pump based on salt hydration/dehydration reactions requires the transport of water vapor from low to high pressure. Alternative compression approaches require condensing of low-pressure water vapor, pumping of liquid water, and subsequent evaporation when the low-side pressure corresponds to sub-ambient water saturation temperatures. Thus, this study compares four steam compression methods for use within a chemical heat pump system based on a reversible calcium oxide hydration/dehydration reaction with a temperature lift from 350 °C heat to >600 °C. Purely mechanical and thermochemical/mechanical compression technologies are considered. A parametric study of maximum allowable temperature, the isentropic efficiency of mechanical compressors, the effectiveness of heat exchangers, and the assumed allowable heat exchanger pressure drop is conducted to determine the mechanical and thermal energy consumed per kilogram of compressed steam. The system complexity in terms of the number of main system components, maximum pressure ratio, and maximum allowable temperature is estimated. Model results show an absorption-based steam compressor has the highest exergetic efficiency for the required chemical heat pump required conditions. As a result, this system configuration was then experimentally demonstrated to illustrate the impact of system performance on component effectiveness.

Advanced reactors↗
DOE OSTI2023

Challenges in correlating oxygen stable isotope ratios of hydrates on uranium ore concentrates to process waters

Exchange of oxygen stable isotopes (δ 18 O values) between precipitation waters and uranium oxides is governed by thermodynamics or kinetics. It has been assumed that meteoric waters can be related to precipitation waters in uranium ore concentrates and their calcination and reduced uranium oxide products. With this assumption, the δ 18 O values of uranium materials could provide forensic signatures that identify the production history and geolocation of nuclear materials. To further exploit the potential of δ 18 O values in nuclear material analysis, this study examines the oxygen stable isotope exchange in two UOCs, magnesium diuranate (MDU) and sodium diuranate (SDU). MDU and SDU were synthesized from solutions of uranyl nitrate hexahydrate using precipitation waters with unique oxygen isotope compositions. The structures of the MDU and SDU were analyzed using powder X-ray diffraction (p-XRD) and thermal mass loss curves, while the δ 18 O values of waters generated during thermal decomposition were analyzed using a thermogravimetric analyzer coupled to an isotope ratio infrared spectrometer (TGA-IRIS). By p-XRD, the MDU was uniform and amorphous across all syntheses with residual crystalline material incorporated as a minor component. Combined with the TGA results, all of the MDU is likely amorphous MgU 2 O 7 ·3H 2 O with MgO impurities present throughout. In contrast, the SDU synthesis resulted in multiple phases with many samples exhibiting crystalline phases including a combination of Na(UO 2 ) 4 O 2 (OH) 5 ·5H 2 O and Na 2 (UO2) 6 O 4 (OH) 6 ·8H 2 O with a Na 2 U 2 O 7 minor phase. A small fraction of the SDU samples were amorphous with no crystalline XRD peaks observed. Mass loss curves of the SDU samples revealed that the amorphous samples contained inclusions of similar crystalline phases compared to the crystalline materials. The uniformity of the MDU samples enabled highly reproducible measurements of δ 18 O values of the water vapor yielded for two dehydration events at 170 °C and 500 °C. In contrast, the multiphase composition of the SDU samples resulted in poor reproducibility in δ 18 O values. In conclusion, neither system revealed any correlation between the δ 18 O values of precipitation water, and the waters released during dehydration of the UOCs.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2026

Raman spectroscopic investigation of ianthinite [U$_2^{4+}$(UO$_2$)$_4$O$_6$(OH)$_4$(H$_2$O)$_4$]·$5$H$_2$O, a rare mixed-valence uranium oxide hydrate

Ianthinite ([[U$_2^{4+}$(UO$_2$)$_4$O$_6$(OH)$_4$(H$_2$O)$_4$]·$5$H$_2$O) is an exotic mineral that possesses U in both tetravalent and hexavalent oxidation states and is structurally related to the U 3 O 8 polymorphs, which are commonly encountered technogenic materials in the nuclear fuel cycle. Despite the similarities between U 3 O 8 and ianthinite, and the importance of ianthinite in U paragenesis, no Raman spectra have been reported for this mineral. Here, to gain a more complete understanding of how structural attributes of ianthinite give rise to observable spectroscopic features and how these may relate to important materials in the nuclear fuel cycle, we provide, for the first time, Raman spectra of ianthinite. Ianthinite readily oxidizes at ambient conditions, complicating analysis of phase-pure material. Several analytical methods are employed herein to decouple the Raman features of ianthinite from its alteration product(s). First, a simple difference spectrum is presented, then results of Raman spectroscopic mapping are employed, and finally, we use a novel processing and analysis method. Each analysis method provides different insight into structural features that are unique to ianthinite, in particular, features that are attributable to U(IV) in distorted octahedral coordination in both ianthinite and U 3 O 8 phases.

Spano, Tyler L. [Oak Ridge National Laboratory (OR↗