Determination of plutonium isotope ratios at very low levels by ICP-MS using on-line electrochemically modulated separations

  • M. Liezers
  • S. A. Lehn
  • K. B. Olsen
  • O. T. FarmerIII
  • Douglas C. Duckworth
Article

Abstract

Electrochemically modulated separations (EMS) are shown to be a rapid and selective means of extracting and concentrating Pu from complex solutions prior to isotopic analysis by inductively coupled plasma mass spectrometry (ICP‐MS). This separation is performed in a flow injection mode, on‐line with the ICP‐MS. A three‐electrode, flow‐by electrochemical cell is used to accumulate Pu at an anodized glassy carbon electrode by redox conversion of Pu(III) to Pu (IV&VI). The entire process takes place in 2% (v/v) (0.46 M) HNO3. No redox chemicals or acid concentration changes are required. Plutonium accumulation and release is redox dependent and controlled by the applied cell potential. Large transient volumetric concentration enhancements can be achieved. Based on more negative U(IV) potentials relative to Pu(IV), separation of Pu from uranium is efficient, thereby eliminating uranium hydride interferences. EMS‐ICP‐MS isotope ratio measurement performance will be presented for femtogram to attogram level plutonium isotope injections.

Keywords

Plutonium Isotopic ICP-MS Quadrupole Electrochemistry Preconcentration Separations Matrix elimination Glassy carbon 

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Copyright information

© Akadémiai Kiadó, Budapest, Hungary 2009

Authors and Affiliations

  • M. Liezers
    • 1
  • S. A. Lehn
    • 1
    • 2
  • K. B. Olsen
    • 1
  • O. T. FarmerIII
    • 1
  • Douglas C. Duckworth
    • 1
  1. 1.Pacific Northwest National LaboratoryRichlandUSA
  2. 2.Champion Technologies Inc.HoustonUSA

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