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Characterization of the behavior and mechanism of electrochemical pre-concentration of plutonium from aqueous solution

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Abstract

Radiochemical analyses usually require sample preparation typically including a pre-concentration step. Previous work was completed showing the success of electrochemical pre-concentration, as applied to 4f-elements, in reducing the time necessary to pre-concentrate a sample. However, these studies did not include the more electrochemically diverse 5f-elements. The objective of this work was to investigate the ability of a multivalent actinide, plutonium (Pu), to be electrochemically pre-concentrated while maximizing the efficiency of the method and proposing a mechanism of pre-concentration. In an aqueous solution with a mercury film electrode, Pu can successfully pre-concentrate and was proposed to do so via amalgamation.

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Acknowledgments

This work is dedicated in loving memory of James O. Schenk. JLD would like to thank Dr. Francis Cheng of the University of Idaho and Dr. Mark Engelmann of Pacific Northwest National Laboratory for their advice and suggestions on the electrochemistry. The authors would like to thank Charles Knaack and Scott Boroughs at the Washington State University GeoAnalytical Laboratory for their assistance in the ICP-MS measurements. JLD would also like to thank Academic Research Initiative of the Joint Domestic Nuclear Detection Office, Department of Homeland Security, and the National Science Foundation, for funding under Grant Numbers ECCS-0833548 and DN-077-ARI-03302. PDA acknowledges support from the US Army, SBC acknowledges support from DHS and NSF as described above, and the Defense Threat Reduction Agency, grant number HDTRA-1-14-10069.

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Authors and Affiliations

  1. Department of Chemistry, Washington State University, Pullman, WA, 99164, USA

    Jamie L. Doyle, James O. Schenk & Sue B. Clark

  2. Office of the Under Secretary of Defense for Policy, Department of Defense, Washington DC, 20301, USA

    Paul D. Schumacher

  3. Los Alamos National Laboratory, MS E554, P.O. Box 1663, Los Alamos, NM, 87545, USA

    Jamie L. Doyle

  4. Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA, 99352, USA

    Sue B. Clark

Authors
  1. Jamie L. Doyle
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  2. Paul D. Schumacher
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  3. James O. Schenk
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  4. Sue B. Clark
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Correspondence to Jamie L. Doyle.

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Doyle, J.L., Schumacher, P.D., Schenk, J.O. et al. Characterization of the behavior and mechanism of electrochemical pre-concentration of plutonium from aqueous solution. J Radioanal Nucl Chem 311, 279–287 (2017). https://doi.org/10.1007/s10967-016-4976-1

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  • DOI: https://doi.org/10.1007/s10967-016-4976-1

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