Highly efficient plutonium scavenging by an extraction chromatography resin containing a tetraaza-12-crown-4 ligand tethered with four diglycolamide pendent arms

Piyali Banerjee, Seraj A. Ansari, Prasanta K. Mohapatra*, Richard J.M. Egberink, Thichur P. Valsala, Darshan B. Sathe, Raj B. Bhatt, Jurriaan Huskens, Willem Verboom

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

1 Citation (Scopus)

Abstract

An efficient extraction chromatography resin, containing tetraaza-12-crown-4 functionalized with four diglycolamide moieties, was evaluated for the separation of plutonium. This chromatography resin yielded very large distribution coefficients for Pu4+ (>105) in 0.5 – 6 M HNO3 feed solutions. Various physicochemical properties such as sorption kinetics, Pu4+ sorption mechanism, and its sorption capacity were investigated. The sorption kinetics, following a pseudo-second-order model, showed that about 10 minutes of equilibration was sufficient for >99.9% sorption of Pu4+. The sorption of Pu4+ on the resin followed the Langmuir monolayer model, which was confirmed by a theoretical calculation based on the kinetic model. The Pu4+ sorption on the resin was driven by a large exothermic enthalpy change (ΔH = −31.4±2.2 kJ/mol) and a positive entropy change (ΔS = 224±15 J/mol/L). The resin could sorb a maximum of 12.1±0.8 mg of Pu per gram of resin, which is equivalent to 1:2 metal/ligand complex on the resin. The Pu4+ from the resin phase was completely stripped with 0.5 M oxalic acid. A possible application of this resin for the separation / pre-concentration of Pu4+ was successfully demonstrated in the column mode.

Original languageEnglish
Article number462419
JournalJournal of chromatography A
Volume1653
Early online date28 Jul 2021
DOIs
Publication statusPublished - 13 Sep 2021

Keywords

  • Actinide
  • Diglycolamide
  • Extraction chromatography
  • Plutonium
  • Separation
  • 22/2 OA procedure

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