Abstract

ABSTRACTRouting neptunium to a single product in spent nuclear fuel reprocessing is a significant challenge. In this work, we have further improved the simulation of neptunium extraction in an advanced PUREX flowsheet by applying a revised model of the Np(V)–Np(VI) redox reaction kinetics, a new nitric acid radiolysis model, and by evaluating various models for the nitrous acid distribution coefficient. The Np disproportionation reaction is shown to have a negligible effect. The models are validated against published ‘cold test’ experimental results; the ‘hot test’ simulation suggests that high neptunium radiolysis could help to achieve high recoveries using this flowsheet.

Highlights

  • Nuclear energy plays an important role in the supply of sustainable and secure electricity

  • The simulation of the hot test shows that the nitrous acid yield through radiolysis can improve the neptunium extraction in the advanced PUREX process and that 99% of neptunium would still be routed to the organic product when radiolysis occurs

  • The hot test simulation results indicate the likely influences of radiolysis on neptunium extraction under radiation conditions that will be present when reprocessing spent nuclear fuel

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Summary

Introduction

Nuclear energy plays an important role in the supply of sustainable and secure electricity. Based on the research of neptunium redox in aqueous-only phase and two-phase extractions,[11,22] a revised description of neptunium kinetics is applied in this work to improve the simulation model. During this reaction, the role of nitrous acid is important: it catalyzes oxidation at low concentrations, but acts as a reductant at high concentrations, reducing Np(VI) to Np(V). The effects of the disproportionation reaction of Np(V) were evaluated and are reported in this article

System overview
Neptunium redox reaction model
Distribution coefficients
Radiolytic yield of nitrous acid
Cold test simulation
Findings
Conclusions
Full Text
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