Contrasting Trivalent Lanthanide and Actinide Complexation by Polyoxometalates via Solution-State NMR
Abstract
Deciphering the solution chemistry and speciation of actinides is inherently difficult due to radioactivity, rarity, and cost constraints, especially for transplutonium elements. In this context, the development of new chelating platforms for actinides and associated spectroscopic techniques is particularly important. In this study, we investigate a relatively overlooked class of chelators for actinide binding, namely, polyoxometalates (POMs). We provide the first NMR measurements on americium–POM and curium–POM complexes, using one-dimensional (1D) 31P NMR, variable-temperature NMR, and spin-lattice relaxation time (T1) experiments. The proposed POM–NMR approach allows for the study of trivalent f-elements even when only microgram amounts are available and in phosphate-containing solutions where f-elements are typically insoluble. The solution-state speciation of trivalent americium, curium, plus multiple lanthanide ions (La3+, Nd3+, Sm3+, Eu3+, Yb3+, and Lu3+), in the presence of the model POM ligand PW11O397– was elucidated and revealed the concurrent formation of two stable complexes, [MIII(PW11O39)(H2O)x]4– and [MIII(PW11O39)2]11–. Interconversion reaction constants, reaction enthalpies, and reaction entropies were derived from the NMR data. The NMR results also provide experimental evidence of the weakly paramagnetic nature of the Am3+ and Cm3+ ions in solution. Furthermore, the study reveals a previously unnoticed periodicity break along the f-element series with the reversal ofmore »
- Authors:
-
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Oregon State University, Corvallis, OR (United States)
- Oregon State University, Corvallis, OR (United States)
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1960017
- Alternate Identifier(s):
- OSTI ID: 1971295
- Report Number(s):
- LLNL-JRNL-837416
Journal ID: ISSN 0020-1669; TRN: US2312930
- Grant/Contract Number:
- NA0003763; AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 62; Journal Issue: 16; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Colla, Christopher A., Colliard, Ian, Sawvel, April M., Nyman, May, Mason, Harris E., and Deblonde, Gauthier J.-P. Contrasting Trivalent Lanthanide and Actinide Complexation by Polyoxometalates via Solution-State NMR. United States: N. p., 2022.
Web. doi:10.1021/acs.inorgchem.2c04014.
Colla, Christopher A., Colliard, Ian, Sawvel, April M., Nyman, May, Mason, Harris E., & Deblonde, Gauthier J.-P. Contrasting Trivalent Lanthanide and Actinide Complexation by Polyoxometalates via Solution-State NMR. United States. https://doi.org/10.1021/acs.inorgchem.2c04014
Colla, Christopher A., Colliard, Ian, Sawvel, April M., Nyman, May, Mason, Harris E., and Deblonde, Gauthier J.-P. Thu .
"Contrasting Trivalent Lanthanide and Actinide Complexation by Polyoxometalates via Solution-State NMR". United States. https://doi.org/10.1021/acs.inorgchem.2c04014. https://www.osti.gov/servlets/purl/1960017.
@article{osti_1960017,
title = {Contrasting Trivalent Lanthanide and Actinide Complexation by Polyoxometalates via Solution-State NMR},
author = {Colla, Christopher A. and Colliard, Ian and Sawvel, April M. and Nyman, May and Mason, Harris E. and Deblonde, Gauthier J.-P.},
abstractNote = {Deciphering the solution chemistry and speciation of actinides is inherently difficult due to radioactivity, rarity, and cost constraints, especially for transplutonium elements. In this context, the development of new chelating platforms for actinides and associated spectroscopic techniques is particularly important. In this study, we investigate a relatively overlooked class of chelators for actinide binding, namely, polyoxometalates (POMs). We provide the first NMR measurements on americium–POM and curium–POM complexes, using one-dimensional (1D) 31P NMR, variable-temperature NMR, and spin-lattice relaxation time (T1) experiments. The proposed POM–NMR approach allows for the study of trivalent f-elements even when only microgram amounts are available and in phosphate-containing solutions where f-elements are typically insoluble. The solution-state speciation of trivalent americium, curium, plus multiple lanthanide ions (La3+, Nd3+, Sm3+, Eu3+, Yb3+, and Lu3+), in the presence of the model POM ligand PW11O397– was elucidated and revealed the concurrent formation of two stable complexes, [MIII(PW11O39)(H2O)x]4– and [MIII(PW11O39)2]11–. Interconversion reaction constants, reaction enthalpies, and reaction entropies were derived from the NMR data. The NMR results also provide experimental evidence of the weakly paramagnetic nature of the Am3+ and Cm3+ ions in solution. Furthermore, the study reveals a previously unnoticed periodicity break along the f-element series with the reversal of T1 relaxation times of the 1:1 and 1:2 complexes and the preferential formation of the long T1 species for the early lanthanides versus the short T1 species for the late lanthanides, americium, and curium. Furthermore, given the broad variety of POM ligands that exist, with many of them containing NMR-active nuclei, the combined POM–NMR approach reported here opens a new avenue to investigate difficult-to-study elements such as heavy actinides and other radionuclides.},
doi = {10.1021/acs.inorgchem.2c04014},
journal = {Inorganic Chemistry},
number = 16,
volume = 62,
place = {United States},
year = {Thu Dec 29 00:00:00 EST 2022},
month = {Thu Dec 29 00:00:00 EST 2022}
}
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