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Immobilization of controlled Pu:Am ratio on actinide-specific affinity monolith support developed in capillary and coupled to inductively coupled plasma mass spectrometry

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Abstract

The objective of this work was to develop an actinide-specific monolithic support in capillary designed to immobilize precise Pu:Am ratios and its coupling to inductively coupled plasma mass spectrometry (ICP-MS) for immobilized metal affinity chromatography applications. This format offers many advantages, such as reducing the sample amount and waste production, which are of prime importance when dealing with highly active radioelements. Four organic phosphorylated-based monoliths were synthesized in situ through UV photo-polymerization in capillary and characterized. The capillary coupling to ICP-MS was set up in conventional laboratory using Th and Sm as chemical analogues of Pu and Am. A dedicated method was developed to quantify online Th and Sm amounts immobilized on the monolithic capillaries, allowing to select the best monolith candidate poly(BMEP-co-EDMA)adp. By precisely adjusting the elemental composition in the loading solutions and applying the developed quantification method, the controlled immobilization of several Th:Sm molar ratios onto the monolith was successful. Finally, the capillary ICP-MS coupling was transposed in a glove box and by applying the strategy developed to design the monolithic support using Th and Sm, the immobilization of a 10.5 ± 0.2 (RSD = 2.3%, n = 3) Pu:Am molar ratio reflecting Pu ageing over 48 years was achieved in a controlled manner on poly(BMEP-co-EDMA)adp. Hence, the new affinity capillary monolithic support was validated, with only hundred nanograms or less of engaged radioelements and can be further exploited to precisely determine differential interactions of Pu and Am with targeted biomolecules in order to better anticipate the effect of Am on Pu biodistribution.

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Acknowledgements

The authors would like to acknowledge the FOCUSDEM R&D program on decommissioning and dismantling of CEA, the French Atomic Energy and Alternative Energies Commission, for financial support. The authors would like to also thank Marina Amaral Saraiva for her support for the setup of the capillary/ICP-MS coupling assembly in the glove box.

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Author notes

  1. Marta Garcia-Cortes

    Present address: Department of Analytical Chemistry, Faculty of Chemistry, Complutense University, Ciudad Universitaria S/N, 28040, Madrid, Spain

Authors and Affiliations

  1. Université Paris-Saclay, CEA, Service de Physico-Chimie, 91191, Gif-Sur-Yvette, France

    Sandra Barhoum, Marta Garcia-Cortes, Marine Boudias, Hélène Isnard, Erwan Dupuis & Carole Bresson

  2. Sorbonne Université, UPMC, 75005, Paris, France

    Sandra Barhoum

  3. Univ Paris Est Créteil, CNRS, ICMPE, UMR 7182, 2 Rue Henri Dunant, 94320, Thiais, France

    Mohamed Guerrouache & Benjamin Carbonnier

  4. Laboratory of Radiotoxicology, CEA, Paris-Saclay University, 91297, Arpajon, France

    Anne Van der Meeren

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Barhoum, S., Garcia-Cortes, M., Boudias, M. et al. Immobilization of controlled Pu:Am ratio on actinide-specific affinity monolith support developed in capillary and coupled to inductively coupled plasma mass spectrometry. Microchim Acta 191, 191 (2024). https://doi.org/10.1007/s00604-024-06274-8

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