<p>The recovery of neptunium (Np) from nuclear waste is of paramount importance for mitigating long-term environmental radiotoxicity. However, this endeavor is significantly hindered by the intricate redox chemistry of Np, which necessitates precise control over its oxidation states. Here we present a straightforward and efficient methodology for the quantitative conversion of Np(V) to Np(IV) under catalysis-free and mild conditions, leveraging organic complexation with an array of widely employed tridentate O-donor ligands: <i>N,N,N</i>’,<i>N</i>’-tetramethyl diglycolamide (TMDGA), <i>N,N</i>-dimethyl diglycolamide (DMDGA), and diglycol acid (DGA). Compared to the “free” Np ion, the reduction efficiency of Np(V) unprecedentedly boosts more than 300 times in the case of complexing with TMDGA, thereby opening up a new path to control the oxidation state of Np and supporting the crucial task of Np recovering in spent nuclear fuel reprocessing.</p>

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A straightforward organic complexation strategy enables precise and efficient oxidation state control of Np

  • Huaixin Hao,
  • Yaoyang Liu,
  • Xue Dong,
  • Yuxiao Guo,
  • Bin Li,
  • Shuang Liu,
  • Chao Xu,
  • Jing Chen,
  • Zhipeng Wang

摘要

The recovery of neptunium (Np) from nuclear waste is of paramount importance for mitigating long-term environmental radiotoxicity. However, this endeavor is significantly hindered by the intricate redox chemistry of Np, which necessitates precise control over its oxidation states. Here we present a straightforward and efficient methodology for the quantitative conversion of Np(V) to Np(IV) under catalysis-free and mild conditions, leveraging organic complexation with an array of widely employed tridentate O-donor ligands: N,N,N’,N’-tetramethyl diglycolamide (TMDGA), N,N-dimethyl diglycolamide (DMDGA), and diglycol acid (DGA). Compared to the “free” Np ion, the reduction efficiency of Np(V) unprecedentedly boosts more than 300 times in the case of complexing with TMDGA, thereby opening up a new path to control the oxidation state of Np and supporting the crucial task of Np recovering in spent nuclear fuel reprocessing.