Developing and downscaling a method by HILIC coupled simultaneously to ESIMS and ICPMS to determine the affinity of lanthanide chelating molecules using specific isotope dilution

文献情報

出版日 2023-10-31

DOI 10.1039/D3JA00263B

インパクトファクター 4.023

著者

Marina Amaral Saraiva, Pascal E. Reiller, Cécile Marie, Carole Bresson

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要旨

Recycling minor actinides (Am, Cm and Np) from spent nuclear fuel is considered by a few countries as an important option for a future sustainable nuclear fuel cycle. For this purpose, solvent extraction processes are developed to separate minor actinides, especially from lanthanides and other fission products. The development of fast and powerful analytical methods is essential to acquire the data needed to model these processes and to improve their performances. For this purpose, this study presents the development, validation and application of a new analytical approach based on the simultaneous coupling of hydrophilic interaction chromatography (HILIC) to electrospray ionization mass spectrometry (ESIMS) and inductively coupled plasma mass spectrometry (ICPMS), using specific isotope dilution (SID) as a method of quantification for the determination of the affinity and selectivity of chelating molecules (TPAEN, NM and DTPA) towards lanthanides (Ln). The best separation conditions of natNd and natSm complexes formed with the three molecules were defined. Then, downscaling the separation was investigated, to reduce effluent volumes, the consumption of materials and the time devoted to experiments which are of concern in the nuclear field. The separation was carried out using an amide grafted stationary phase column in isocratic and gradient elution modes depending on the separation format. The separated complexes were online identified and the quantitative distribution of the Ln among the complexes was simultaneously determined owing to our quantification strategy. The results obtained were similar for the three separation formats, allowing us to validate the robustness of the method. By applying this method, the affinity of TPAEN, NM and DTPA present in competition for the complexation reaction with natNd and natSm was further determined in a single step, allowing a quick screening. Both selectivity and affinity of these molecules could be compared to select the most promising candidates. This approach can be advantageously extended to the evaluation of the affinity of various classes of chelating molecules used in very low quantities, towards elements of interest in the fields of energy, toxicology and the environment.

掲載誌

Journal of Analytical Atomic Spectrometry

CiteScore: 6.2

自己引用率: 25.8%

年間論文数: 254

The Journal of Analytical Atomic Spectrometry (JAAS) is the central journal for publishing innovative research on fundamentals, instrumentation, and methods in the determination, speciation and isotopic analysis of (trace) elements within all fields of application. This includes, but is not restricted to, the most recent progress, developments and achievements in all forms of atomic and elemental detection, isotope ratio determination, molecular analysis, plasma-based analysis and X-ray techniques. The journal welcomes full papers, communications, technical notes, critical and tutorial review articles, editorials, and comments, in addition to the Atomic Spectrometry Updates (ASU) literature reviews that are prepared by an expert panel. Submissions are welcome in the following areas, but note this list reflects the current scope and authors are strongly encouraged to contact the Editorial team if they believe that their work offers potentially new and emerging research relevant to the journal remit: Fundamental studies in the following. New and existing sources for atomic emission, absorption, fluorescence and mass spectrometry and those that provide both atomic and molecular information Sample introduction techniques for solids, liquids, gases Improvements in sensitivity, selectivity, precision, accuracy and/or robustness Isotope ratio measurements, including techniques for improving precision and mass bias correction Single channel and multichannel simultaneous detection systems Chemometrics, statistics, calibration techniques and internal standardisation Theoretical and numerical modelling of fundamental processes related to all of the above methodologies Novel or improved methodologies in areas of application including, but not limited to the following. Biosciences, including elemental, speciation and isotopic analysis in biological systems, immunoassays based on metal-labeled antibodies, bio-imaging, and nanoparticle toxicology Geochemistry Environmental science Materials science, including engineered nanoparticles and quantum dots Metrology, including reference materials Forensic analysis Food and agricultural sciences Energy Archaeometry Molecular analysis. Molecular sources for elemental and isotopic analysis Atomic sources for molecular analysis Atomic and molecular techniques simultaneously used for complementary chemical information All contributions are judged on originality and quality of scientific content, and appropriateness of length to content of new science.