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Title: Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution

Abstract

The peroxydisulfate anion has long been used for the preparation of hexavalent americium (Am VI) from the normally stable Am III valence state in mildly acidic solutions. However, there has been no satisfactory means to directly prepare the pentavalent state (Am V) in that medium. Some early literature reports indicated that the peroxydisulfate oxidation was incomplete, and silver ion catalysis in conjunction with peroxydisulfate became accepted as the means to ensure quantitative generation of Am VI. Incomplete oxidation would be expected to leave residual Am III, or to produce Am V in treated solutions. However, until recently, the use of peroxydisulfate as an Am V reagent has not been reported. Here, parameters influencing the oxidation were investigated, including peroxydisulfate and acid concentration, temperature, duration of oxidative treatment, and the presence of higher concentrations of other redox active metals such as plutonium. Using optimized conditions determined here, quantitative Am V was prepared in an acidic solution and the UV/Vis extinction coefficients of the Am V 513 nm peak were measured over a range of nitric acid concentrations. Furthermore, the utility of Am V for separations from the lanthanides and curium by solvent extraction, organic column chromatography and inorganic ion exchangers wasmore » also investigated.« less

Authors:
 [1];  [1];  [1];  [2];  [2]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
  2. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1252474
Report Number(s):
SRNL-STI-2015-00142
Journal ID: ISSN 2046-2069; RSCACL
Grant/Contract Number:  
AC09-08SR22470
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
RSC Advances
Additional Journal Information:
Journal Volume: 5; Journal Issue: 34; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English

Citation Formats

Mincher, Bruce J., Schmitt, Nicholas C., Schuetz, Brian K., Shehee, Thomas C., and Hobbs, David T.. Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution. United States: N. p., 2015. Web. doi:10.1039/C5RA03196F.
Mincher, Bruce J., Schmitt, Nicholas C., Schuetz, Brian K., Shehee, Thomas C., & Hobbs, David T.. Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution. United States. doi:10.1039/C5RA03196F.
Mincher, Bruce J., Schmitt, Nicholas C., Schuetz, Brian K., Shehee, Thomas C., and Hobbs, David T.. Wed . "Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution". United States. doi:10.1039/C5RA03196F. https://www.osti.gov/servlets/purl/1252474.
@article{osti_1252474,
title = {Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution},
author = {Mincher, Bruce J. and Schmitt, Nicholas C. and Schuetz, Brian K. and Shehee, Thomas C. and Hobbs, David T.},
abstractNote = {The peroxydisulfate anion has long been used for the preparation of hexavalent americium (AmVI) from the normally stable AmIII valence state in mildly acidic solutions. However, there has been no satisfactory means to directly prepare the pentavalent state (AmV) in that medium. Some early literature reports indicated that the peroxydisulfate oxidation was incomplete, and silver ion catalysis in conjunction with peroxydisulfate became accepted as the means to ensure quantitative generation of AmVI. Incomplete oxidation would be expected to leave residual AmIII, or to produce AmV in treated solutions. However, until recently, the use of peroxydisulfate as an AmV reagent has not been reported. Here, parameters influencing the oxidation were investigated, including peroxydisulfate and acid concentration, temperature, duration of oxidative treatment, and the presence of higher concentrations of other redox active metals such as plutonium. Using optimized conditions determined here, quantitative AmV was prepared in an acidic solution and the UV/Vis extinction coefficients of the AmV 513 nm peak were measured over a range of nitric acid concentrations. Furthermore, the utility of AmV for separations from the lanthanides and curium by solvent extraction, organic column chromatography and inorganic ion exchangers was also investigated.},
doi = {10.1039/C5RA03196F},
journal = {RSC Advances},
number = 34,
volume = 5,
place = {United States},
year = {Wed Mar 11 00:00:00 EDT 2015},
month = {Wed Mar 11 00:00:00 EDT 2015}
}

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