Development of quantitative analytical methods for the control of actinides in a pyrochemical partitioning process

Abstract

Summary Advanced nuclear fuel cycles are being developed in order to reduce the long-term radiotoxicity of highly radioactive waste. Pyrochemical partitioning techniques appear particularly attractive for advanced fuel cycles in which the minor actinides are recycled. The electrochemical processes of practical importance are the electrorefining process and the liquid–liquid extraction of transuranic (TRU) elements from fission products using either non-miscible molten metal or molten salt–metal phases. Analytical methods for the accurate assay of actinide elements in these matrices needed to be developed. A quantitative assay is required in order to establish a material balance for process development and – at a later stage – for accountancy and control purposes. To this end radiometric techniques such as energy-dispersive X-ray fluorescence analysis (XRF), neutron coincidence counting (NCC) and high-resolution gamma spectrometry (HRGS) were extensively employed for the quantitative determination of actinides (U, Np, Pu, Am, Cm) in process samples. Comparative analyses were performed using inductively coupled plasma mass spectrometry (ICP-MS). The respective samples were available in small quantities (≅100 mg) either in the form of eutectic salt or in metallic form with Cd, Zr or Bi as major metallic matrix constituents.