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Title: The coordination chemistry of Cm III , Am III , and Ac III in nitrate solutions: an actinide L 3 -edge EXAFS study

Abstract

Understanding actinide(III) (AnIII = CmIII, AmIII, AcIII) solution-phase speciation is critical for controlling many actinide processing schemes, ranging from medical applications to reprocessing of spent nuclear fuel. Unfortunately, in comparison to most elements in the periodic table, AnIII speciation is often poorly defined in complexing aqueous solutions and in organic media. This neglect – in large part – is a direct result of the radioactive properties of these elements, which make them difficult to handle and acquire. Here in this paper, we surmounted some of the handling challenges associated with these exotic 5f-elements and characterized CmIII, AmIII, and AcIII using AnIII L3-edge X-ray absorption spectroscopy (XAS) as a function of increasing nitric acid (HNO3) concentration. Our results revealed that actinide aquo ions, An(H2O)x3+ (x = 9.6 ± 0.7, 8.9 ± 0.8, and 10.0 ± 0.9 for CmIII, AmIII, and AcIII), were the dominant species in dilute HNO3 (0.05 M). In concentrated HNO3 (16 M), shell-by-shell fitting of the extended X-ray fine structure (EXAFS) data showed the nitrate complexation increased, such that the average stoichiometries of Cm(NO3)4.1±0.7(H2O)5.7±1.3(1.1±0.2)-, Am(NO3)3.4±0.7(H2O)5.4±0.5(0.4±0.1)-, and Ac(NO3)2.3±1.7(H2O)8.3±5.2(0.7±0.5)+ were observed. Data obtained at the intermediate HNO3 concentration (4 M) were modeled as a linear combination of the 0.05 andmore » 16 M spectra. Here, for all three metals, the intermediate models showed larger contributions from the 0.05 M HNO3 spectra than from the 16 M HNO3 spectra. Additionally, these efforts enabled the Cm–NO3 and Ac–NO3 distances to be measured for the first time. Moreover, the AnIII L3-edge EXAFS results, contribute to the growing body of knowledge associated with CmIII, AmIII, and AcIII coordination chemistry, in particular toward advancing understanding of AnIII solution phase speciation.« less

Authors:
 [1];  [1];  [1];  [1];  [2]; ORCiD logo [1];  [3];  [1];  [4]
  1. Los Alamos National Laboratory,, USA
  2. Los Alamos National Laboratory,, USA, Department of Physics, University of Washington, Seattle
  3. Stanford University, USA
  4. Department of Physics, University of Washington, Seattle, USA
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1462444
Alternate Identifier(s):
OSTI ID: 1463561
Report Number(s):
LA-UR-18-22688
Journal ID: ISSN 2041-6520; CSHCBM
Grant/Contract Number:  
20180005DR; AC52-06NA25396; AC02-76SF00515
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 9 Journal Issue: 35; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ferrier, Maryline G., Stein, Benjamin W., Bone, Sharon E., Cary, Samantha K., Ditter, Alexander S., Kozimor, Stosh A., Lezama Pacheco, Juan S., Mocko, Veronika, and Seidler, Gerald T. The coordination chemistry of Cm III , Am III , and Ac III in nitrate solutions: an actinide L 3 -edge EXAFS study. United Kingdom: N. p., 2018. Web. doi:10.1039/C8SC02270D.
Ferrier, Maryline G., Stein, Benjamin W., Bone, Sharon E., Cary, Samantha K., Ditter, Alexander S., Kozimor, Stosh A., Lezama Pacheco, Juan S., Mocko, Veronika, & Seidler, Gerald T. The coordination chemistry of Cm III , Am III , and Ac III in nitrate solutions: an actinide L 3 -edge EXAFS study. United Kingdom. doi:10.1039/C8SC02270D.
Ferrier, Maryline G., Stein, Benjamin W., Bone, Sharon E., Cary, Samantha K., Ditter, Alexander S., Kozimor, Stosh A., Lezama Pacheco, Juan S., Mocko, Veronika, and Seidler, Gerald T. Mon . "The coordination chemistry of Cm III , Am III , and Ac III in nitrate solutions: an actinide L 3 -edge EXAFS study". United Kingdom. doi:10.1039/C8SC02270D.
@article{osti_1462444,
title = {The coordination chemistry of Cm III , Am III , and Ac III in nitrate solutions: an actinide L 3 -edge EXAFS study},
author = {Ferrier, Maryline G. and Stein, Benjamin W. and Bone, Sharon E. and Cary, Samantha K. and Ditter, Alexander S. and Kozimor, Stosh A. and Lezama Pacheco, Juan S. and Mocko, Veronika and Seidler, Gerald T.},
abstractNote = {Understanding actinide(III) (AnIII = CmIII, AmIII, AcIII) solution-phase speciation is critical for controlling many actinide processing schemes, ranging from medical applications to reprocessing of spent nuclear fuel. Unfortunately, in comparison to most elements in the periodic table, AnIII speciation is often poorly defined in complexing aqueous solutions and in organic media. This neglect – in large part – is a direct result of the radioactive properties of these elements, which make them difficult to handle and acquire. Here in this paper, we surmounted some of the handling challenges associated with these exotic 5f-elements and characterized CmIII, AmIII, and AcIII using AnIII L3-edge X-ray absorption spectroscopy (XAS) as a function of increasing nitric acid (HNO3) concentration. Our results revealed that actinide aquo ions, An(H2O)x3+ (x = 9.6 ± 0.7, 8.9 ± 0.8, and 10.0 ± 0.9 for CmIII, AmIII, and AcIII), were the dominant species in dilute HNO3 (0.05 M). In concentrated HNO3 (16 M), shell-by-shell fitting of the extended X-ray fine structure (EXAFS) data showed the nitrate complexation increased, such that the average stoichiometries of Cm(NO3)4.1±0.7(H2O)5.7±1.3(1.1±0.2)-, Am(NO3)3.4±0.7(H2O)5.4±0.5(0.4±0.1)-, and Ac(NO3)2.3±1.7(H2O)8.3±5.2(0.7±0.5)+ were observed. Data obtained at the intermediate HNO3 concentration (4 M) were modeled as a linear combination of the 0.05 and 16 M spectra. Here, for all three metals, the intermediate models showed larger contributions from the 0.05 M HNO3 spectra than from the 16 M HNO3 spectra. Additionally, these efforts enabled the Cm–NO3 and Ac–NO3 distances to be measured for the first time. Moreover, the AnIII L3-edge EXAFS results, contribute to the growing body of knowledge associated with CmIII, AmIII, and AcIII coordination chemistry, in particular toward advancing understanding of AnIII solution phase speciation.},
doi = {10.1039/C8SC02270D},
journal = {Chemical Science},
number = 35,
volume = 9,
place = {United Kingdom},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/C8SC02270D

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Cited by: 7 works
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Figures / Tables:

Fig. 1 Fig. 1 : The background subtracted and normalized room temperature solution-phase AnIII L3-edge XANES spectra of AnIII (An = CmIII, top; AmIII, middle; AcIII, bottom) cations dissolved in HNO3 (0.05 M, blue trace; 4 M, red trace; and 16 M, green trace). Spectra are displayed with a slight y-offset formore » clarity.« less

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