U.S. Department of EnergyOffice of Scientific and Technical Information
Ion association with tetra-n-alkylammonium cations stabilizes higher-oxidation-state neptunium dioxocations
Abstract
Extended–coordination sphere interactions between dissolved metals and other ions, including electrolyte cations, are not known to perturb the electrochemical behavior of metal cations in water. Herein, we report the stabilization of higher–oxidation state Np dioxocations in aqueous chloride solutions by hydrophobic tetra-nalkylammonium (TAA+) cations—an effect not exerted by fully hydrated Li+ cations under similar conditions. Experimental and molecular dynamics simulation results indicate that TAA+ cations not only drive enhanced coordination of anionic Cl– ligands to NpV/VI but also associate with the resulting Np complexes via non-covalent interactions, which together decrease the electrode potential of the NpVI/NpV couple by up to 220 mV (ΔΔG = –22.2 kJ mol–1). Understanding the solvation–dependent interplay between electrolyte cations and metal–oxo species opens an avenue for controlling the formation and redox properties of metal complexes in solution. As a result, it also provides valuable mechanistic insights into actinide separation processes that widely use quaternary ammonium cations as extractants or in room temperature ionic liquids.
- Authors:
-
[1];
[2];
[3]
- Argonne National Lab. (ANL), Argonne, IL (United States); Clemson Univ., Anderson, SC (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); 3M Corporate Research Analytical Lab., St. Paul, MN (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1494551
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Estes, Shanna L., Qiao, Baofu, and Jin, Geng Bang. Ion association with tetra-n-alkylammonium cations stabilizes higher-oxidation-state neptunium dioxocations. United States: N. p., 2019.
Web. doi:10.1038/s41467-018-07982-5.
Estes, Shanna L., Qiao, Baofu, & Jin, Geng Bang. Ion association with tetra-n-alkylammonium cations stabilizes higher-oxidation-state neptunium dioxocations. United States. https://doi.org/10.1038/s41467-018-07982-5
Estes, Shanna L., Qiao, Baofu, and Jin, Geng Bang. 2019.
"Ion association with tetra-n-alkylammonium cations stabilizes higher-oxidation-state neptunium dioxocations". United States. https://doi.org/10.1038/s41467-018-07982-5. https://www.osti.gov/servlets/purl/1494551.
@article{osti_1494551,
title = {Ion association with tetra-n-alkylammonium cations stabilizes higher-oxidation-state neptunium dioxocations},
author = {Estes, Shanna L. and Qiao, Baofu and Jin, Geng Bang},
abstractNote = {Extended–coordination sphere interactions between dissolved metals and other ions, including electrolyte cations, are not known to perturb the electrochemical behavior of metal cations in water. Herein, we report the stabilization of higher–oxidation state Np dioxocations in aqueous chloride solutions by hydrophobic tetra-nalkylammonium (TAA+) cations—an effect not exerted by fully hydrated Li+ cations under similar conditions. Experimental and molecular dynamics simulation results indicate that TAA+ cations not only drive enhanced coordination of anionic Cl– ligands to NpV/VI but also associate with the resulting Np complexes via non-covalent interactions, which together decrease the electrode potential of the NpVI/NpV couple by up to 220 mV (ΔΔG = –22.2 kJ mol–1). Understanding the solvation–dependent interplay between electrolyte cations and metal–oxo species opens an avenue for controlling the formation and redox properties of metal complexes in solution. As a result, it also provides valuable mechanistic insights into actinide separation processes that widely use quaternary ammonium cations as extractants or in room temperature ionic liquids.},
doi = {10.1038/s41467-018-07982-5},
url = {https://www.osti.gov/biblio/1494551},
journal = {Nature Communications},
issn = {2041-1723},
number = 1,
volume = 10,
place = {United States},
year = {Fri Jan 04 00:00:00 EST 2019},
month = {Fri Jan 04 00:00:00 EST 2019}
}
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Figures / Tables:
Fig. 1: Effect of Li+ vs. [NMe4]+ on the NpVI/NpV couple. Currentnormalized cyclic voltammetry data for solutions of 5 mM NpV dissolved in 5M NMe4Cl or 5 M LiCl at pH ≈ 1.3. The arrow indicates the initial scan direction. Initial and cathodic switching potential= 400/550mV; anodic switching potential= 1000/1150mV;more »
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Impacts of hydrogen bonding interactions with Np( v / vi )O 2 Cl 4 complexes: vibrational spectroscopy, redox behavior, and computational analysis
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Enhancing Metal Separations Using Hydrophilic Ionic Liquids and Analogues as Complexing Agents in the More Polar Phase of Liquid–Liquid Extraction Systems
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