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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Countercurrent Actinide Lanthanide Separation Process (ALSEP) Demonstration Test with a Simulated PUREX Raffinate in Centrifugal Contactors on the Laboratory Scale

An Actinide Lanthanide Separation Process (ALSEP) for the separation of trivalent actinides (An(III)) from simulated raffinate solution was successfully demonstrated using a 32-stage 1 cm annular centrifugal contactor setup. The ALSEP solvent was composed of a mixture of 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) and N,N,N',N'-tetra-(2-ethylhexyl)-diglycolamide (T2EHDGA) in n-dodecane. Flowsheet calculations and evaluation of the results were done using the Argonne’s Model for Universal Solvent Extraction (AMUSE) code using single-stage distribution data. The co-extraction of Zr(IV) and Pd(II) was prevented using CDTA (trans-1,2-diaminocyclohexane-N,N,N',N'-tetraacetic acid) as a masking agent in the feed. For the scrubbing of co-extracted Mo; citrate-buffered acetohydroxamic acid was used. The separation of An(III) from the trivalent lanthanides (Ln(III)) was achieved using citrate-buffered diethylene-triamine-N,N,N',N",N"-pentaacetic acid (DTPA), and Ln(III) were efficiently back extracted using N,N,N',N'-tetraethyl-diglycolamide (TEDGA). A clean An(III) product was obtained with a recovery of 95% americium and curium. The Ln(III) were efficiently stripped; but the Ln(III) product contained 5% of the co-stripped An(III). The carryover of Am and Cm into the Ln(III) product is attributed to too few actinide stripping stages, which was constrained by the number of centrifugal contactors available. Improved separation would be achieved by increasing the number of An strip stages. The heavier lanthanides (Pr, Nd, Sm, Eu, and Gd) and yttrium were mainly routed to the Ln product, whereas the lighter lanthanides (La and Ce) were mostly routed to the raffinate.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Organic Speciation and Interactions in ALSEP. One Step Partitioning Process of MinorActinides, Lanthanides, and Fission Products

Research conducted in this project focused on speciation characterization of the ALSEP extraction system (similar to the TALSPEAK-like application) which addresses recovery of minor actinides and lanthanides from PUREX raffinate. The ALSEP (Actinide-Lanthanide Separation) system proposes a trivalent minor actinide/lanthanide group extraction followed by a selective actinide strip to effectively partition minor actinides, lanthanides, and other fission products. The group extraction is achieved by a mixed organic solvent, combining acidic and neutral extracting ligands. The objective of this work is investigation the interactions of the acidic and neutral ligands with each other in the extraction organic solvent and with desired metals. Four combinations of a cation-exchange ligand (either HDEHP or HEH[EHP]) and a neutral solvating ligand (either TODGA or T2EHDGA) in n-dodecane were studied. Interligand dimers in these combinations were investigated with NMR and FTIR, the strongest interaction was observed for HDEHP+TODGA and weakest for T2EHDGA+HEH[EHP]. Complexes of the trivalent Am and lanthanides Nd, Eu, Ho, Pr in these binary ligand mixtures were probed with spectroscopic (UV–vis, time-resolved fluorescence, XAFS and SAXS-spectroscopies) and extraction (Job’s plot, slope analysis) methods; co-extracted water and nitric acid were analyzed by titration methods. Comparison of the collected spectra showed significant shifting for both DGA ligands with HDEHP, while both combinations of HEH[EHP]+DGA displayed much smaller spectral changes. Data were modeled with HypSpec program, and stability constants for extracted complexes were calculated. Aggregation in these systems were studied by SAXS (small-angle X-ray scattering) spectroscopy and interfacial tension, size of aggregates were measured. Two PhD students graduated (2017, 2018) and one student continues her PhD study.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1974

Cold cathode gauge experiment (ALSEP)

Cold cathode ionization gages were left on the lunar surface as part of ALSEP (Apollo Lunar Surface Experiment Package) on Apollo missions 12, 14, and 15. An instrument prepared for Apollo 13 did not reach the surface because of the abort of that mission. The gages that reached the lunar surface measured the amounts of gas present in the vicinity of the ALSEP sites. The observed daytime gas concentrations were initially about two orders of magnitude greater than the nighttime observations; this was due to contamination of the landing area by the Apollo operations and equipment, and the daytime measurements showed a decrease with time characterized by a time constant of a few months.

Johnson, F. S.↗
NASA NTRS2018

History and Status of ALSEP and the Apollo Lunar Data Project

A suite of automated scientific instruments (the Apollo Lunar Surface Experiment Package, or ALSEP) was installed at each of the landing sites of Apollo 12, 14, 15, 16, and 17 from 1969 to 1972. They operated from deployment until decommissioning on 30 September 1977. These data were continuously transmitted to Earth and saved on the Range Tapes, which were recorded at the Manned Space Flight Network stations. These data were also broken out by experiment and sent to the experiment Principal Investigators on what were called the P.I. Tapes. Starting in April 1973 the Range Tape data were stored in digital format on 7-track magnetic tapes, the ARCSAV Tapes. In February 1976, the handling of the Range Tapes was transferred to UT Galveston. They produced 9-track tapes referred to as the Work Tapes. Following the Apollo program the Range and ARCSAV tapes, which were never archived, were lost. The Work Tapes were archived at the National Space Science Data Center (NSSDC). Some investigators archived their individual experiment data with NSSDC as well, but much of the data had minimal documentation, were not in digital form, or were stored in difficult to translate formats. Data from many experiments were never delivered to the NSSDC. The Lunar Data Project was started to address the problem of both missing and not readily usable data. Our effort has resulted in recovery of some of the ARCSAV tapes, recovery and digitization of a large volume of Apollo scientific and technical documentation, and restoration of many ALSEP and other Apollo data collections. Restoration involves deciphering formats, assembling necessary ancillary data (metadata), and packaging data in digital format to be archived with the Planetary Data System (PDS). Recovery of the data from the ARCSAV tapes involved having the tapes read on special equipment and extracting the individual experiment data out of the integrated data stream. We will report on the history and status of the various recovery efforts.

Work Tapes↗
DOE OSTI2016

Accomplishing Equilibrium in ALSEP: Demonstrations of Modified Process Chemistry on 3-D Printed Enhanced Annular Centrifugal Contactors

Here, the major components of the modified ALSEP process have been demonstrated on a modified 2-cm annular centrifugal contactor with an enhanced mixing zone using stable fission products and radiotracers. The results show that by decreasing the pH of the minor actinide stripping solution, using HEDTA instead of DTPA, and increasing contact time, the process is very effective in separating americium from the lanthanides and the fission products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Actinide Lanthanide Separation Process – ALSEP

Separation of the minor actinides (Am, Cm) from the lanthanides at an industrial scale remains a significant technical challenge for closing the nuclear fuel cycle. To increase the safety of used nuclear fuel (UNF) reprocessing, as well as reduce associated costs, a novel solvent extraction process has been developed. The process allows for partitioning minor actinides, lanthanides and fission products following uranium/plutonium/neptunium removal; minimizing the number of separation steps, flowsheets, chemical consumption, and waste. This new process, Actinide Lanthanide SEParation (ALSEP), uses an organic solvent consisting of a neutral diglycolamide extractant, either N,N,N',N'-tetra(2 ethylhexyl)diglycolamide (T2EHDGA) or N,N,N',N'-tetraoctyldiglycolamide (TODGA), and an acidic extractant 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]), dissolved in an aliphatic diluent (e.g. n-dodecane). The An/Ln co-extraction is conducted from moderate-to-strong nitric acid, while the selective stripping of the minor actinides from the lanthanides is carried out using a polyaminocarboxylic acid/citrate buffered solution at pH anywhere between 3 and 4.5. The extraction and separation of the actinides from the fission products is very effective in a wide range of HNO3 concentrations and the minimum separation factors for lanthanide/Am exceed 30 for Nd/Am, reaching > 60 for Eu/Am under some conditions. The experimental results presented here demonstrate the great potential for a combined system, consisting of a neutral extractant such as T2EHDGA or TODGA, and an acidic extractant such as HEH[EHP], for separating the minor actinides from the lanthanides.

actinide separation↗
DOE OSTI2023

Low and High LET Degradation Studies of Metal-Loaded Organic Phase Ligands in the ALSEP Process

Organic solutions comprising the Actinide Lanthanide Separation Process (ALSEP) solvent consisting of 0.5 M 2-ethylhexyl phosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) and 0.05 M N,N,N’,N’-tetra(2-ethylhexyl)diglycolamide (T2EHDGA) in n-dodecane were subjected to low LET and high LET irradiation before and after equilibration with an aqueous phase of 3 M HNO 3 . Degradation dose constants revealed greater ligand degradation due to gamma irradiation than alpha irradiation for both ligands. Furthermore, equilibration with nitric acid did not have a significant impact on ligand degradation for either irradiation source. Identified degradation products were similar for both gamma and alpha irradiation and occurred mostly through the rupture of the N–C carbonyl and C–O ether bonds for T2EHDGA and the C–Oether bond in HEH[EHP]. Acid contact appears to alter the degradation pathway by favoring the formation of higher molecular weight recombination products. Furthermore, mixed T2EHDGA-HEH[EHP]-NO 3 complexes were formed with Nd(III) after extraction from 3 M HNO 3 , and low LET gamma irradiation of the Nd(III) loaded organic solution produced similar degradation products as the organic solution absent of Nd(III). Interestingly, and likely due to the greater radiolytic susceptibility of T2EHDGA than HEH[EHP], a HEH[EHP]-Nd(III) complex appears to form as the T2EHDGA degrades with increasing absorbed dose.

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

Project 18-15263 X-ray Studies of Interfacial Molecular Complexes in ALSEP Back-Extraction (Research Performance Final Report)

The objective of the project was to use synchrotron X-rays to measure the molecular-scale organization of extractants, complexants, buffers, and metal ions at the organic-aqueous (liquid-liquid) interface during solvent back-extraction under conditions relevant to ALSEP (Actinide-Lanthanide Separation Process). The capability of X-ray fluorescence near total reflection (XFNTR) was extended to explore the distribution of Eu(III) between the liquid-liquid interface and bulk organic and aqueous phases which contained extractants HDEHP (bis(2-ethylhexyl) phosphoric acid) and HEHEHP (2-ethylhexyl phosphonic acid mono-2-ethylhexyl ester), the complexant DTPA (diethylene triamine pentaacetic acid), and citric and nitric acids. Although an Am-compatible sample cell was developed, extending x-ray measurements of flat liquid-liquid interfaces to the actinide Am(III) did not prove to be possible within constraints imposed by the Advanced Photon Source. However, preliminary measurements with a drop cell may eventually provide a path forward to investigate Am(III) at a liquid interface. It was also demonstrated that competitive binding that occurs during back-extraction of lanthanide ions to either a phosphoric acid extractant (DHDP, di-hexadecyl phosphate) at the liquid interface or to complexant DTPA in the bulk aqueous phase could be reversibly tuned by X-ray exposure. Separately, X-ray measurements from the liquid-vapor interface explored the role of the aqueous solubility of HDEHP and HEHEHP and their interactions with a range of lanthanides and transition metal ions. Finally, the capability of X-ray absorption spectroscopy (EXAFS) was extended to probe metal ion coordination in lanthanide ion-extractant complexes at the liquid-vapor interface. Complementary to the specific interfacial systems studied during this project, the development of x-ray techniques expands our ability to understand ion ordering at liquid interfaces.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1972

FCC for ALSEP (lunar experiment)

The use of FCC in the ALSEP is discussed. Cable requirements, tradeoffs with round wire, design and development problems are described.

Cripps, G.↗
NASA NTRS1975

Precision selenodesy and lunar libration through VLBI observations of ALSEPs

Data from 500 observation series, each one representing about five hours' continuous observation of a pair of ALSEPs by differential very long baseline interferometers (VLBI) have been compiled on magnetic tape. The theoretical models used to calculate the rotation of the earth, the orbit of the moon, the libration of the moon, and the basic VLBI observable were improved substantially. Analysis of data from long spans of VLBI observations was begun.

Counselman, C. C., III↗
NASA NTRS1977

VLBI Observations of ALSEP Transmitters

The technique of differential very-long-baseline inteferometry (VLBI) Apollo Lunar Surface Experiments Package was used to measure the relative positions of the (ALSEP) transmitters at the Apollo 12, 14, 15, 16, and 17 lunar landing sites with uncertainties less than 0.005 sec of the geocentric arc. These measurements yielded improved determinations of the selenodetic coordinates of the Apollo landing sites, and of the physical libration of the moon.

Counselman, C. C.↗
NASA NTRS2014

Shadowing on Apollo 12 Solar Cells and Possible Movement of the ALSEP Central Station

A fortuitous arrangement of a west-facing solar cell and a bracket on the Apollo 12 ALSEP (Apollo Lunar Surface Experiments Package) has allowed us to precisely determine the relative position of the Sun near sunset relative to the Apollo 12 central station over a period of nearly 8 years. The small bracket, mounted on the central station due west of the cell, casts a shadow on the cell near sunset, decreasing the output of the cell proportional to the area of shadow covering the cell. The pattern of shadowing by the bracket gives good agreement with the known change of solar azimuth on a yearly timescale, but the pattern gradually but constantly changed from year-to-year, in a manner inconsistent with the known and changing position of the Sun.

Apollo↗