MINIATURIZED EXTRACTION DEVICE COUPLED TO MASS SPECTROMETRY FOR ON-LINE PURIFICATION AND CHARACTERIZATION OF NUCLEAR SAMPLES - CEA - Commissariat à l’énergie atomique et aux énergies alternatives Accéder directement au contenu
Communication Dans Un Congrès Année : 2024

MINIATURIZED EXTRACTION DEVICE COUPLED TO MASS SPECTROMETRY FOR ON-LINE PURIFICATION AND CHARACTERIZATION OF NUCLEAR SAMPLES

Résumé

Characterizing the elemental and isotopic composition of nuclear samples is of utmost importance in the case of nuclear forensics, processes for spent fuel recycling or waste treatment. Protocols already exist for extraction of radionuclides such as U and Pu using cartridges packed with commercial resins before off-line characterization by Inductively Coupled Plasma Mass Spectrometry (ICP-MS). Current methods are however time-consuming, induce exposition of operators to variable levels of radiation, and the production of large amounts of waste. In this study, we developed a miniaturized extraction device and its coupling to ICP-MS in order to reduce the scale and drawbacks of the current purification steps. Gao et al. [1] and Ouchi et al. [2] designed resin-packed microchannels and were able to carry out the off-line analysis of U or Th separated from trace elements, but the repeatability of the packing process and the performance of the separation have yet to be confirmed. Porous monoliths with larger surface area than particulate phases can be directly integrated within microdevices and represent a more convenient approach. In this sense, two routes were investigated by our group through the post-functionalization of a generic monolith in cyclic olefin copolymer (COC) microsystems, using either grafting [3] or impregnation techniques [4] but exhibit limitations. Our new integrated strategy consists in the one step synthesis of a monolith dedicated to U/Pu isolation by copolymerization of phosphorylated monomers in the channels of a COC microsystem and in its coupling to ICP-MS, that was not developed in the previous works. Optimization of monoliths compositions in relation with their permeability, morphology, extraction capacity, and selectivity properties was first realized in silica capillaries since the activation/anchoring step is well known for this material compared to COC. All monoliths were synthesized by photopolymerization. Figure 1 shows the UV collimated LED specifically set up in the laboratory to limit diffusion effects in comparison with traditional UV oven. The coupling of the functionalized capillaries to ICP-MS was performed (Figure 2) and ad-hoc quantification methods developed to determine the loading capacity of U either alone or in the presence of Th and Sm used as Pu and Am analogues (Figure 3). Several mobile phase compositions were considered for the selective retention and elution of the elements. The development of these different steps in a conventional laboratory is essential to validate the separation downscaling before performing the purification of radioactive samples, which requires the transposition of the methodology in a glove box. Once the most promising monolith was selected, we worked on the implementation of the synthesis and anchorage in the channels of COC microsystems, with particular attention paid to the repeatability of the method. One and two-steps photochemically induced activation methods were compared. Among all parameters tested, the type of photoinitiator, the time and power of irradiation had the most prominent effects on monolith anchoring. The sorbent volume in the proposed microdevice should be reduced at most by a factor of 10,000 compared to conventional methods. Word Count: 489
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Dates et versions

cea-04288524 , version 1 (16-11-2023)

Identifiants

  • HAL Id : cea-04288524 , version 1

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Marine Boudias, Erwan Dupuis, Alexandre Quemet, Carole Bresson. MINIATURIZED EXTRACTION DEVICE COUPLED TO MASS SPECTROMETRY FOR ON-LINE PURIFICATION AND CHARACTERIZATION OF NUCLEAR SAMPLES. MicroTAS 2023, Oct 2023, Katowice, Poland. ⟨cea-04288524⟩
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