The vaporisation behaviour of americium dioxide by use of mass spectrometry

Gotcu-Freis, P.; Colle, Jean‐Yves; Hiernaut, J.-P.; Konings, R.J.M.

doi:10.1016/j.jnucmat.2010.12.024

Cited by 15 publications

(19 citation statements)

References 16 publications

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“…When the low values of the oxygen potential in the region 1.5 < O/Am < 1.7 as found by Otobe et al [29] were imposed in the optimisation, the miscibility gap found by Sari [9] could not be described. Furthermore the calculated americium oxide vapour pressure data above AmO 2 samples were found inconsistent with our experiments [11] in that case. Therefore the phase boundary data for the sesquioxide were given higher weight than the measurements of oxygen potentials close to O/Am = 1.5.…”

Section: Am-o Systemcontrasting

confidence: 98%

“…Furthermore, the experimental high partial pressures of Am(g) could not be reproduced by our calculations in the single phase AmO 2Àx or in the two-phase region (AmO 2Àx + AmO 1.62 ). Finally, a reasonable agreement (P calc /P exp % 10) between the calculated partial pressures for Am(g), AmO(g), AmO 2 (g) and the recent experimental data measured by mass spectrometry in [11] is found for the congruency calculation above the sesquioxide phase Am 2 O 3 (Fig. 10).…”

Section: Am-o Systemsupporting

confidence: 75%

“…Due to the large discrepancy at a low O/Am ratios, a selection of these data was made. Although an attempt was performed to fit the recent oxygen potential data measured by Otobe et al [29], the results were not reasonable with the existing phase diagram data and the vapour pressure measurements performed over AmO 2 samples previously [11]. Therefore a higher weighting was given therefore to the phase boundary functions of the sesquioxide.…”

Section: Discussionmentioning

confidence: 85%

“…Calculations of the vapour pressure data in the Am-O system were performed for comparison with the recent experimental results measured by mass spectrometry [11]. The final O/Am ratio of the sample could not be measured, due to the small amount material used and its dispersed state (fine powder).…”

Section: Am-o Systemmentioning

confidence: 99%

“…Using the fragmentation patterns obtained in previous studies on pure plutonium dioxide [10] and on americium dioxide [11] samples, the signal intensities were corrected for dissociation processes occurring at 40 eV, and the contribution of each species in the vapour was evaluated. Thus for congruency at T = 2300 K the vapour consists of 73% PuO 2 and 27% PuO with respect to the total plutonium oxide pressure, P(Pu tot ), and 46% AmO, 41% AmO 2 and 13% Am, with respect to the total americium oxide pressure, P(Am tot ).…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

A thermodynamic study of the Pu–Am–O system

Gotcu-Freis

Colle

Guéneau

et al. 2011

Journal of Nuclear Materials

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Section: Am-o Systemcontrasting

confidence: 98%

Section: Am-o Systemsupporting

confidence: 75%

Section: Discussionmentioning

confidence: 85%

Section: Am-o Systemmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

A thermodynamic study of the Pu–Am–O system

Gotcu-Freis

Colle

Guéneau

et al. 2011

Journal of Nuclear Materials

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An original approach for Raman spectroscopy analysis of radioactive materials and its application to americium‐containing samples

Naji

Colle

Beneš

et al. 2015

J Raman Spectroscopy

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An approach for Raman measurements of highly radioactive samples is presented here. The innovative part of this approach lies in the fact that no single part of the Raman equipment is in direct contact with the radioactive sample, as the sample is sealed in an alphatight capsule. Raman analysis is effectively performed through the optical-grade quartz window closing the capsule. This allows performing micro-Raman measurements on radioactive samples with no limitations on the laser source wavelength, polarisation mode, spectrometer mode and microscope mode (provided the focal length of the microscope objective is greater than the thickness of the quartz window and with sub mg samples). Some example results are shown and discussed. In particular, some spectral features of americium-containing oxide nuclear fuel specimens are presented. Raman spectra clearly reveal in these specimens the presence of abundant oxygen defects induced in the fcc fluorite lattice by trivalent americium. In order to complete the analysis the Raman spectrum of pure americium dioxide was also measured with a lower energy excitation source compared with previous research. The current results seem to be consistent with the possible occurrence of a photolysis process induced by the Raman laser, resulting in the formation of hyperstoichiometric americium sesquioxide Am 2 O 3 + z . Such a photolytic process is deemed to be unavoidable when visible lasers are used as excitation sources for the Raman analysis of americium dioxide.

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A review on the mass spectrometric studies of americium: Present status and future perspective

Aggarwal

2016

Mass Spectrometry Reviews

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The manuscript reviews the various mass spectrometric techniques for analysis and chemical studies of Americium. These methods include thermal ionization mass spectrometry (TIMS), and inductively coupled plasma source mass spectrometry (ICPMS) for the determination of Am isotope ratios and concentration in nuclear fuel samples of interest in nuclear technology, and in complex biological and environmental samples. Ultra-sensitive mass spectrometric techniques of resonance-ionization mass spectrometry (RIMS), and accelerator-based mass spectrometry (AMS) are also discussed. The novel applications of electrospray ionization mass spectrometry (ESIMS) to understand the solution chemistry of Am and other actinides are presented. These studies are important in view of the world-wide efforts to develop novel complexing agents to separate lanthanides and minor actinides (Am, Np, and Cm) for partitioning and transmutation of minor actinides from the point of view of nuclear waste management. These mass spectrometry experiments are also of great interest to examine the covalent character of actinides with increasing atomic number. Studies on gas-phase chemistry of Am and its oxides with Knudsen effusion mass spectrometry (KEMS), Fourier-transform ion cyclotron resonance mass spectrometry (FTICR-MS), and laser-based experiments with reflectron time-of-flight mass spectrometer (R-ToF) are highlighted. These studies are important to understand the fundamental chemistry of 5f electrons in actinides. Requirement of certified isotopic reference materials of Am to improve the accuracy of experimental nuclear data (e.g., the half-life of Am) is emphasized. © 2016 Wiley Periodicals, Inc. Mass Spec Rev.

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The vaporisation behaviour of americium dioxide by use of mass spectrometry

Cited by 15 publications

References 16 publications

A thermodynamic study of the Pu–Am–O system

A thermodynamic study of the Pu–Am–O system

An original approach for Raman spectroscopy analysis of radioactive materials and its application to americium‐containing samples

A review on the mass spectrometric studies of americium: Present status and future perspective

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