Modulating the Ce(III)/Ce(IV) redox potential via chelation for the separation of Ce(IV) from Pr(III) by solvent extraction.

Authors

Xiang Li, Hu Song, Chenchen Yuan, Qingye Zhou, Shufeng Zhao, Wanjun Mu, Zeng Huang, Jun Tu, Xingliang Li

Published in

Dalton transactions (Cambridge, England : 2003). Sep 07, 2026. Epub Sep 07, 2026.

Abstract

Carrier-free ¹⁴³Pr is a promising radionuclide for bone pain palliation. However, its selective separation from neutron-irradiated cerium targets remains challenging, primarily due to the nearly identical aqueous chemistry of Ce(III) and Pr(III). Here, we present a coupled strategy that integrates coordination-regulated valence-state control with synergistic solvent extraction. 2,6-Pyridinedicarboxylic acid (DPA) is employed as a multidentate ligand to selectively stabilise Ce(IV) through strong coordination. This valence transformation is systematically validated by potentiometry, single-crystal X-ray diffraction, cyclic voltammetry, and X-ray photoelectron spectroscopy. Building on this, a 4,4,4-trifluoro-1-phenylbutane-1,3-dione (HBTA)/trioctylphosphine oxide (TOPO) extraction system is introduced to achieve selective separation of Pr(III). The results demonstrate that the HBTA/TOPO system exhibits a pronounced preference for Ce(IV) over Pr(III), with significantly enhanced separation factors across a broad pH range. This strategy provides a viable chemical route to produce high-purity carrier-free ¹⁴³Pr from irradiated cerium targets. More broadly, it establishes a general framework for the selective separation of adjacent light lanthanides through coordination-mediated redox control.

PMID:
42704356
Bibliographic data and abstract were imported from PubMed on 07 Sep 2026.

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