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- Horne, Gregory P., et al.
(author)
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Effect of chemical environment on the radiation chemistry of N,N-di-(2-ethylhexyl)butyramide (DEHBA) and plutonium retention
- 2019
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In: Dalton Transactions. - : ROYAL SOC CHEMISTRY. - 1477-9226 .- 1477-9234. ; 48:38, s. 14450-14460
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Journal article (peer-reviewed)abstract
- N,N-di-(2-ethylhexyl)butyramide (DEHBA) has been proposed as part of a hydro-reprocessing solvent extraction system for the co-extraction of uranium and plutonium from spent nuclear fuel, owing to its selectivity for hexavalent uranium and tetravalent plutonium. However, there is a critical lack of quantitative understanding regarding the impact of chemical environment on the radiation chemistry of DEHBA, and how this would affect process performance. Here we present a systematic investigation into the radiolytic degradation of DEHBA in a range of n-dodecane solvent system formulations, where we subject DEHBA to gamma irradiation, measure reaction kinetics, ligand integrity, degradation product formation, and investigate solvent system performance through uranium and plutonium extraction and strip distribution ratios. The rate of DEHBA degradation in n-dodecane was found to be slow (G = -0.31 +/- 0.02 mu mol J(-1)) but enhanced upon contact with the oxidizing conditions of the investigated solvent systems (organic-only, or in contact with either 0.1 or 3.0 M aqueous nitric acid). Two major degradation products were identified in the organic phase, bis-2-ethylhexylamine (b2EHA) and N-(2-ethylhexyl)butyramide (MEHBA), resulting from the cleavage of C-N bonds, and could account for the total loss of DEHBA up to similar to 300 kGy for organic-only conditions. Both b2EHA and MEHBA were also found to be susceptible to radiolytic degradation, having G-values of -0.12 +/- 0.01 and -0.08 +/- 0.01 mu mol J(-1), respectively. Solvent extraction studies showed: (i) negligible change in uranium extraction and stripping with increasing absorbed dose; and (ii) plutonium extraction and retention exhibits complex dependencies on absorbed dose and chemical environment. Organic-only conditions afforded enhanced plutonium extraction and retention attributed to b2EHA, while acid contacts inhibited this effect and promoted significant plutonium retention for the highest acidity. Overall it has been demonstrated that chemical environment during irradiation has a significant influence on the extent of DEHBA degradation and plutonium retention.
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- Villebrun, F., et al.
(author)
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Magnetic fields of intermediate-mass T Tauri stars : I. Magnetic detections and fundamental stellar parameters
- 2019
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In: Astronomy and Astrophysics. - : EDP Sciences. - 0004-6361 .- 1432-0746. ; 622
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Journal article (peer-reviewed)abstract
- Context. The origin of the fossil magnetic fields detected in 5 to 10% of intermediate-mass main sequence stars is still highly debated.Aims. We want to bring observational constraints to a large population of intermediate-mass pre-main sequence (PMS) stars in order to test the theory that convective-dynamo fields generated during the PMS phases of stellar evolution can occasionally relax into fossil fields on the main sequence.Methods. Using distance estimations, photometric measurements, and spectropolarimetric data from HARPSpol and ESPaDOnS of 38 intermediate-mass PMS stars, we determined fundamental stellar parameters (T-eff, L and v sin i) and measured surface magnetic field characteristics (including detection limits for non-detections, and longitudinal fields and basic topologies for positive detections). Using PMS evolutionary models, we determined the mass, radius, and internal structure of these stars. We compared different PMS models to check that our determinations were not model-dependant. We then compared the magnetic characteristics of our sample accounting for their stellar parameters and internal structures.Results. We detect magnetic fields in about half of our sample. About 90% of the magnetic stars have outer convective envelopes larger than similar to 25% of the stellar radii, and heavier than similar to 2% of the stellar mass. Going to higher mass, we find that the magnetic incidence in intermediate-mass stars drops very quickly, within a timescale on the order of few times 0.1 Myr. Finally, we propose that intermediate-mass T Tauri stars with large convective envelopes, close to the fully convective limit, have complex fields and that their dipole component strengths may decrease as the sizes of their convective envelopes decrease, similar to lower-mass T Tauri stars.
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