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Title: Self-irradiation and oxidation effects on americium sesquioxide and Raman spectroscopy studies of americium oxides

Abstract

Americium oxides samples were characterized by X-ray diffraction (XRD) and Raman spectroscopy, with an emphasis on their structural behavior under oxidation and self-irradiation. Raman spectra of americium dioxide (AmO{sub 2}) and sesquioxide (Am{sub 2}O{sub 3}) were obtained for the first time. With the help of literature data on isostructural oxides, Raman signatures of Ia-3 C-type Am{sub 2}O{sub 3} and P-3m1 A-type Am{sub 2}O{sub 3} are identified. For AmO{sub 2,} a clear band is noted at 390 cm{sup −1}. Its nature is compared to that of the other actinide dioxides. Am{sub 2}O{sub 3} evolution under ambient conditions and against {sup 241}Am α self-irradiation was monitored by powder XRD. The sample, initially composed of A-type Am{sub 2}O{sub 3} as major phase as well as C2/m B-type and C-type structures as minor phases, progressively oxidizes to Fm-3m AmO{sub 2−δ} over a few months. On the basis of diffractogram refinements, evolutions of unit cell volumes caused by self-irradiation are also determined and discussed. - Graphical abstract: The evolution of americium oxide under ambient conditions was monitored using XRD (X-ray diffraction) and Raman spectroscopy. After a thermal treatment under reducing conditions, a polyphasic sample mainly composed of A- and C-type americium sesquioxides is evidenced bymore » XRD and Raman spectroscopy. The sample then evolves through two processes: oxidation and self-irradiation. The first one provokes the progressive appearance of F-type americium dioxide while the initial phases disappear, whereas the main effect of the second is a structural swelling with time. - Highlights: • The first Raman spectroscopy measurements on americium oxides were performed. • Observed Am{sub 2}O{sub 3} Raman bands were identified thanks to data on analogue compounds. • AmO{sub 2} assumed T{sub 2g} band presents a shift compared to the actinide dioxide series. • Am{sub 2}O{sub 3} evolution under self-irradiation and oxidation was also monitored by XRD. • The three Am{sub 2}O{sub 3} phases observed have different behaviors under self-irradiation.« less

Authors:
 [1];  [2];  [1];  [2];  [3];  [1]
  1. CEA, DEN, DTEC/SDTC/LEMA, F-30207 Bagnols-sur-Cèze Cedex (France)
  2. CEA, DEN, DTCD/SECM/LMPA, F-30207 Bagnols-sur-Cèze Cedex (France)
  3. Unité de Catalyse et Chimie du Solide, UMR 8012 CNRS, Ecole Nationale Supérieure de Chimie de Lille BP 90108, 59652 Villeneuve d’Ascq Cedex (France)
Publication Date:
OSTI Identifier:
22443399
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 217; Other Information: Copyright (c) 2014 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; AMERICIUM; AMERICIUM OXIDES; HEAT TREATMENTS; MONITORS; OXIDATION; PHASE TRANSFORMATIONS; POWDERS; RAMAN SPECTRA; RAMAN SPECTROSCOPY; SELF-IRRADIATION; X-RAY DIFFRACTION

Citation Formats

Horlait, Denis, Caraballo, Richard, Lebreton, Florent, Jégou, Christophe, Roussel, Pascal, and Delahaye, Thibaud, E-mail: thibaud.delahaye@cea.fr. Self-irradiation and oxidation effects on americium sesquioxide and Raman spectroscopy studies of americium oxides. United States: N. p., 2014. Web. doi:10.1016/J.JSSC.2014.05.025.
Horlait, Denis, Caraballo, Richard, Lebreton, Florent, Jégou, Christophe, Roussel, Pascal, & Delahaye, Thibaud, E-mail: thibaud.delahaye@cea.fr. Self-irradiation and oxidation effects on americium sesquioxide and Raman spectroscopy studies of americium oxides. United States. doi:10.1016/J.JSSC.2014.05.025.
Horlait, Denis, Caraballo, Richard, Lebreton, Florent, Jégou, Christophe, Roussel, Pascal, and Delahaye, Thibaud, E-mail: thibaud.delahaye@cea.fr. Mon . "Self-irradiation and oxidation effects on americium sesquioxide and Raman spectroscopy studies of americium oxides". United States. doi:10.1016/J.JSSC.2014.05.025.
@article{osti_22443399,
title = {Self-irradiation and oxidation effects on americium sesquioxide and Raman spectroscopy studies of americium oxides},
author = {Horlait, Denis and Caraballo, Richard and Lebreton, Florent and Jégou, Christophe and Roussel, Pascal and Delahaye, Thibaud, E-mail: thibaud.delahaye@cea.fr},
abstractNote = {Americium oxides samples were characterized by X-ray diffraction (XRD) and Raman spectroscopy, with an emphasis on their structural behavior under oxidation and self-irradiation. Raman spectra of americium dioxide (AmO{sub 2}) and sesquioxide (Am{sub 2}O{sub 3}) were obtained for the first time. With the help of literature data on isostructural oxides, Raman signatures of Ia-3 C-type Am{sub 2}O{sub 3} and P-3m1 A-type Am{sub 2}O{sub 3} are identified. For AmO{sub 2,} a clear band is noted at 390 cm{sup −1}. Its nature is compared to that of the other actinide dioxides. Am{sub 2}O{sub 3} evolution under ambient conditions and against {sup 241}Am α self-irradiation was monitored by powder XRD. The sample, initially composed of A-type Am{sub 2}O{sub 3} as major phase as well as C2/m B-type and C-type structures as minor phases, progressively oxidizes to Fm-3m AmO{sub 2−δ} over a few months. On the basis of diffractogram refinements, evolutions of unit cell volumes caused by self-irradiation are also determined and discussed. - Graphical abstract: The evolution of americium oxide under ambient conditions was monitored using XRD (X-ray diffraction) and Raman spectroscopy. After a thermal treatment under reducing conditions, a polyphasic sample mainly composed of A- and C-type americium sesquioxides is evidenced by XRD and Raman spectroscopy. The sample then evolves through two processes: oxidation and self-irradiation. The first one provokes the progressive appearance of F-type americium dioxide while the initial phases disappear, whereas the main effect of the second is a structural swelling with time. - Highlights: • The first Raman spectroscopy measurements on americium oxides were performed. • Observed Am{sub 2}O{sub 3} Raman bands were identified thanks to data on analogue compounds. • AmO{sub 2} assumed T{sub 2g} band presents a shift compared to the actinide dioxide series. • Am{sub 2}O{sub 3} evolution under self-irradiation and oxidation was also monitored by XRD. • The three Am{sub 2}O{sub 3} phases observed have different behaviors under self-irradiation.},
doi = {10.1016/J.JSSC.2014.05.025},
journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = ,
volume = 217,
place = {United States},
year = {2014},
month = {9}
}