Dataset Information

Ultra-selective ligand-driven separation of strategic actinides.

ABSTRACT: Metal ion separations are critical to numerous fields, including nuclear medicine, waste recycling, space exploration, and fundamental research. Nonetheless, operational conditions and performance are limited, imposing compromises between recovery, purity, and cost. Siderophore-inspired ligands show unprecedented charge-based selectivity and compatibility with harsh industry conditions, affording excellent separation efficiency, robustness and process control. Here, we successfully demonstrate a general separation strategy on three distinct systems, for Ac, Pu, and Bk purification. Separation factors (SF) obtained with model compound 3,4,3-LI(1,2-HOPO) are orders of magnitude higher than with any other ligand currently employed: 10⁶ between Ac and relevant metal impurities, and over 10⁸ for redox-free Pu purification against uranyl ions and trivalent actinides or fission products. Finally, a one-step separation method (SF > 3 × 10⁶ and radiopurity > 99.999%) enables the isolation of Bk from adjacent actinides and fission products. The proposed approach offers a paradigm change for the production of strategic elements.

SUBMITTER: Deblonde GJ

PROVIDER: S-EPMC6547845 | biostudies-literature | 2019 Jun

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

Ultra-selective ligand-driven separation of strategic actinides.

Deblonde Gauthier J-P GJ Ricano Abel A Abergel Rebecca J RJ

Nature communications 20190604 1

Metal ion separations are critical to numerous fields, including nuclear medicine, waste recycling, space exploration, and fundamental research. Nonetheless, operational conditions and performance are limited, imposing compromises between recovery, purity, and cost. Siderophore-inspired ligands show unprecedented charge-based selectivity and compatibility with harsh industry conditions, affording excellent separation efficiency, robustness and process control. Here, we successfully demonstrate a ...[more]

PMID: 31164638

Similar Datasets

Project description:Separation of lanthanides (Ln) from actinides (An) is unanimously challenging in reprocessing used nuclear fuel despite of much dedicated efforts over the past several decades. The TALSPEAK process is the current reference method in the United States for Ln3+/An3+ separation but suffers from several limitations, such as a narrow working pH window (3.5-4.0), costly pH buffers, and slow extraction kinetics. Studies aiming at improving TALSPEAK have so far focused on polyaminocarboxylates hold-back reagents. Here, a new class of water-soluble ligands comprising hydroxypyridinone metal-binding units are evaluated for Ln3+/An3+ separation. The model octadentate chelator 3,4,3-LI(1,2-HOPO) (abbreviated as HOPO) was used in combination with several industry-relevant organic extractants to separate Gd from four transplutonium elements (Am, Cm, Bk, and Cf). Cyanex 301 GN and HDEHP worked best in combination with HOPO, whereas HEH[EHP], Cyanex 572, and ACORGA M5640 did not yield practical Ln3+/An3+ separation. Separation factors between Gd3+ and Am3+ reach about 50 with the HOPO/Cyanex 301 GN system and 30 with the HOPO/HDEHP system. The results using HDEHP (SFGd/Am = 30, SFGd/Cm = 8.5, and SFGd/Cf = 773) are high enough for industrial applications, and the proposed system works at pH values as low as 1.5, which simplifies the process by eliminating the need for pH buffers. In contrast to previously proposed methods, the HOPO-based process is also highly selective at separating Bk from Ln3+ (SFGd/Bk = 273) owing to in situ, spontaneous oxidation of Bk(III) to Bk(IV) by HOPO. The optimal pH in the case of HOPO/Cyanex 301 GN is 3.6 (SFAm/Gd = 50, SFCm/Gd = 23, SFBk/Gd = 1.4, and SFCf/Gd = 3.2), but this system has the advantage of extracting An ions into the organic phase while keeping Ln ions in the aqueous phase, which is opposite to the conventional TALSPEAK process. This study represents the first optimization of a TALSPEAK-like Ln/An separation method using a HOPO chelator and paves the avenue for further developments of analytical science and reprocessing of used nuclear fuel.

Dataset Information

Ultra-selective ligand-driven separation of strategic actinides.

Publications

Ultra-selective ligand-driven separation of strategic actinides.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets