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Next-Generation 3,3′-AlkoxyBTPs as Complexants for Minor Actinide Separation from Lanthanides: A Comprehensive Separations, Spectroscopic, and DFT Study

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Inorg. Chem. 2024, 63, 11, 4819-4827
    Article

    Next-Generation 3,3′-AlkoxyBTPs as Complexants for Minor Actinide Separation from Lanthanides: A Comprehensive Separations, Spectroscopic, and DFT Study
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    • Lesta S. Fletcher
      Lesta S. Fletcher
      Department of Chemistry, Tennessee Technological University, Cookeville, Tennessee 38505-0001, United States
      More by Lesta S. Fletcher
      Orcidhttps://orcid.org/0000-0003-2185-848X
    • Mariah L. Tedder
      Mariah L. Tedder
      Department of Chemistry, Tennessee Technological University, Cookeville, Tennessee 38505-0001, United States
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    • Samiat O. Olayiwola
      Samiat O. Olayiwola
      Department of Chemistry, Tennessee Technological University, Cookeville, Tennessee 38505-0001, United States
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    • Nickolas A. Joyner
      Nickolas A. Joyner
      Department of Chemistry, The University of Alabama, Tuscaloosa, Alabama 35487, United States
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    • Marcos M. Mason
      Marcos M. Mason
      Department of Chemistry, The University of Alabama, Tuscaloosa, Alabama 35487, United States
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    • Allen G. Oliver
      Allen G. Oliver
      Department of Chemistry, The University of Notre Dame, Notre Dame, Indiana 46656, United States
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      Orcidhttps://orcid.org/0000-0002-0511-1127
    • Dale D. Ensor
      Dale D. Ensor
      Department of Chemistry, Tennessee Technological University, Cookeville, Tennessee 38505-0001, United States
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    • David A. Dixon
      David A. Dixon
      Department of Chemistry, The University of Alabama, Tuscaloosa, Alabama 35487, United States
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      Orcidhttps://orcid.org/0000-0002-9492-0056
    • Jesse D. Carrick*
      Jesse D. Carrick
      Department of Chemistry, Tennessee Technological University, Cookeville, Tennessee 38505-0001, United States
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0002-0663-2426
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2024, 63, 11, 4819–4827
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    https://doi.org/10.1021/acs.inorgchem.3c02061
    Published March 4, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Progress toward the closure of the nuclear fuel cycle can be achieved if satisfactory separation strategies for the chemoselective speciation of the trivalent actinides from the lanthanides are realized in a nonproliferative manner. Since Kolarik’s initial report on the utility of bis-1,2,4-triazinyl-2,6-pyridines (BTPs) in 1999, a perfect complexant-based, liquid–liquid separation system has yet to be realized. In this report, a comprehensive performance assessment for the separation of 241Am3+ from 154Eu3+ as a model system for spent nuclear fuel using hydrocarbon-actuated alkoxy-BTP complexants is described. These newly discovered complexants realize gains that contemporary aryl-substituted BTPs have yet to achieve, specifically: long-term stability in highly concentrated nitric acid solutions relevant to the low pH of unprocessed spent nuclear fuel, high DAm over DEu in the economical, nonpolar diluent Exxal-8, and the demonstrated capacity to complete the separation cycle with high efficiency by depositing the chelated An3+ to the aqueous layer via decomplexation of the metal–ligand complex. These soft-N-donor BTPs are hypothesized to function as bipolar complexants, effectively traversing the organic/aqueous interface for effective chelation and bound metal/ligand complex solubility. Complexant design, separation assays, spectroscopic analysis, single-crystal X-ray crystallographic data, and DFT calculations are reported.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.3c02061.

    • Raw data for separations and spectroscopic studies, statistical analysis, single-crystal X-ray diffraction data, and copies of 1H and 13C NMR spectra for new compounds (PDF)

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    CCDC 2267981 contains the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2024, 63, 11, 4819–4827
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.3c02061
    Published March 4, 2024
    Copyright © 2024 American Chemical Society
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