EWCPS 2025 - 20th European Winter Conference on Plasma Spectrochemistry
Lecture
04.03.2025
Experiences in method development of ultra-trace 237Np measurements using MC-ICP-MS in the absence of a 236Np tracer
SP

Sophie Page (Ph.D.)

AWE

Page, S. (Speaker)¹; Dunne, J.¹; Gilligan, C.¹; Jiang, J.¹; Stow, M.¹
¹AWE, Reading (United Kingdom)
Vorschau
20 Min. Untertitel (CC)

Quantification of 237Np is required for environmental monitoring, waste characterisation, and nuclear forensics. Isotope dilution mass spectrometry (IDMS) is an established measurement method that the Radiochemistry community uses for assay of trace-level analytes (< 1 μg). IDMS requires a sample and an isotopic spike of known molality to be weighed with a high degree of precision, mixed, equilibrated, and then measured. The preferred isotope dilution tracer for 237Np quantification is 236Np. However, there are no commercially available 236Np or other appropriate isotope tracers of suitable purity and traceability, which is a chronic issue for the Radioanalytical Chemistry community [1].

This presentation outlines alternative approaches and corresponding recommendations for measurement of 237Np where a suitable 236Np tracer is not available (Figure 1). Specifically, the production and calibration of 239Np for chemical yielding, chemical yielding measurements by gamma spectrometry, separation of 237Np from sample matrix, and a comparison of multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) measurement techniques that do not require 236Np. These techniques include external calibration and IDMS using 233U as a tracer.

Method validation data from NIST Standard Reference Material 4341a and NPL Neptunium-237 Standard Solution R21-04-2020020437-1/A200005 are presented that demonstrate measurement accuracy at the sub-picogram level (< 1 × 10-12 g) with estimated relative uncertainties of \(\sim \) 3 % (k = 1). Finally, the application of these measurements is discussed in the context of recent plutonium radiochronometry work (237Np/241Pu atom ratio) from our laboratory [2], lower-level environmental samples (Standard Reference Material NIST 4350B, Columbia River Sediment), and a recent blind inter-laboratory comparison exercise.

[1] S.M. Jerome, K. Carney, R. Essex, M.E. Fassbender, S. Goldberg, M. Kinlaw, S.P. LaMont, D. Mackney, J.J. Morrison, F.M. Nortier Reference materials for neptunium determination, 2017, 126, 44-48.

[2] M.A. Higginson, J.A. Dunne, C.R.D. Gilligan, S.T.J. Cross, S. Dunn, Z. Varga, Application of plutonium radiochronometry to the analysis of plutonium age dating reference materials, 2022, 331, 3591-3600.

Abstract

Abstract

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