In:
Dalton Transactions, Royal Society of Chemistry (RSC), Vol. 50, No. 43 ( 2021), p. 15576-15584
Kurzfassung:
Efficient separation of neptunium and plutonium from spent nuclear fuel is essential for advanced nuclear fuel cycles. At present, the development of effective actinide separation ligands has become a top priority. As common adsorbents for extracting uranium from seawater, amidoxime-based adsorbents may also be able to separate actinides from high-level liquid waste (HLLW). In this work, the complexation of Np( iv , v , vi ) and Pu( iv ) and alkyl chains (R = C 13 H 26 ) modified with amidoximate (AO − ) and carboxyl (Ac − ) functional groups was systematically studied by quantum chemical calculations. For all the studied complexing species, the RAc − and RAO − ligands act as monodentate or bidentate ligands. Complexes with AO − groups show higher covalency of the metal–ligand bonding than the analogues with Ac − groups, in line with the binding energy analysis. Bonding analysis verifies that these amidoxime/carboxyl-based adsorbents possess higher coordination affinity toward Pu( iv ) than toward Np( iv ), and the Np( vi ) complexes have stronger covalent interactions than Np( v ). According to thermodynamic analysis, these adsorbents have the ability to separate Np( iv , v , vi ) and Pu( iv ), and also exhibit potential performance for partitioning Pu( iv ) from Np( iv ) under acidic conditions. This work can help to deeply understand the interaction between transuranium elements and amidoxime-based adsorbents, and provide a theoretical basis for the separation of actinides with amidoxime-based adsorbents.
Materialart:
Online-Ressource
ISSN:
1477-9226
,
1477-9234
Sprache:
Englisch
Verlag:
Royal Society of Chemistry (RSC)
Publikationsdatum:
2021
ZDB Id:
1472887-4
