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.
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| Title: | 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. |
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| Authors: | Amaral Saraiva, Marina1 (AUTHOR), Reiller, Pascal E.1 (AUTHOR), Marie, Cécile2 (AUTHOR), Bresson, Carole1 (AUTHOR) carole.bresson@cea.fr |
| Source: | JAAS (Journal of Analytical Atomic Spectrometry). Dec2023, Vol. 38 Issue 12, p2674-2690. 17p. |
| Subjects: | Hydrophilic interaction liquid chromatography, Rare earth metals, Inductively coupled plasma mass spectrometry, Solvent extraction, Fuel cycle, Isotope dilution analysis, Electrospray ionization mass spectrometry, Molecules |
| Abstract: | 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. [ABSTRACT FROM AUTHOR] |
| Copyright of JAAS (Journal of Analytical Atomic Spectrometry) is the property of Royal Society of Chemistry and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.) | |
| Database: | Engineering Source |
| FullText | Text: Availability: 0 |
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| Header | DbId: egs DbLabel: Engineering Source An: 173928842 AccessLevel: 6 PubType: Academic Journal PubTypeId: academicJournal PreciseRelevancyScore: 0 |
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| Items | – Name: Title Label: Title Group: Ti Data: 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. – Name: Author Label: Authors Group: Au Data: <searchLink fieldCode="AR" term="%22Amaral+Saraiva%2C+Marina%22">Amaral Saraiva, Marina</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Reiller%2C+Pascal+E%2E%22">Reiller, Pascal E.</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Marie%2C+Cécile%22">Marie, Cécile</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Bresson%2C+Carole%22">Bresson, Carole</searchLink><relatesTo>1</relatesTo> (AUTHOR)<i> carole.bresson@cea.fr</i> – Name: TitleSource Label: Source Group: Src Data: <searchLink fieldCode="JN" term="%22JAAS+%28Journal+of+Analytical+Atomic+Spectrometry%29%22">JAAS (Journal of Analytical Atomic Spectrometry)</searchLink>. Dec2023, Vol. 38 Issue 12, p2674-2690. 17p. – Name: Subject Label: Subjects Group: Su Data: <searchLink fieldCode="DE" term="%22Hydrophilic+interaction+liquid+chromatography%22">Hydrophilic interaction liquid chromatography</searchLink><br /><searchLink fieldCode="DE" term="%22Rare+earth+metals%22">Rare earth metals</searchLink><br /><searchLink fieldCode="DE" term="%22Inductively+coupled+plasma+mass+spectrometry%22">Inductively coupled plasma mass spectrometry</searchLink><br /><searchLink fieldCode="DE" term="%22Solvent+extraction%22">Solvent extraction</searchLink><br /><searchLink fieldCode="DE" term="%22Fuel+cycle%22">Fuel cycle</searchLink><br /><searchLink fieldCode="DE" term="%22Isotope+dilution+analysis%22">Isotope dilution analysis</searchLink><br /><searchLink fieldCode="DE" term="%22Electrospray+ionization+mass+spectrometry%22">Electrospray ionization mass spectrometry</searchLink><br /><searchLink fieldCode="DE" term="%22Molecules%22">Molecules</searchLink> – Name: Abstract Label: Abstract Group: Ab Data: 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. [ABSTRACT FROM AUTHOR] – Name: AbstractSuppliedCopyright Label: Group: Ab Data: <i>Copyright of JAAS (Journal of Analytical Atomic Spectrometry) is the property of Royal Society of Chemistry and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.) |
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| RecordInfo | BibRecord: BibEntity: Identifiers: – Type: doi Value: 10.1039/d3ja00263b Languages: – Code: eng Text: English PhysicalDescription: Pagination: PageCount: 17 StartPage: 2674 Subjects: – SubjectFull: Hydrophilic interaction liquid chromatography Type: general – SubjectFull: Rare earth metals Type: general – SubjectFull: Inductively coupled plasma mass spectrometry Type: general – SubjectFull: Solvent extraction Type: general – SubjectFull: Fuel cycle Type: general – SubjectFull: Isotope dilution analysis Type: general – SubjectFull: Electrospray ionization mass spectrometry Type: general – SubjectFull: Molecules Type: general Titles: – TitleFull: 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. Type: main BibRelationships: HasContributorRelationships: – PersonEntity: Name: NameFull: Amaral Saraiva, Marina – PersonEntity: Name: NameFull: Reiller, Pascal E. – PersonEntity: Name: NameFull: Marie, Cécile – PersonEntity: Name: NameFull: Bresson, Carole IsPartOfRelationships: – BibEntity: Dates: – D: 01 M: 12 Text: Dec2023 Type: published Y: 2023 Identifiers: – Type: issn-print Value: 02679477 Numbering: – Type: volume Value: 38 – Type: issue Value: 12 Titles: – TitleFull: JAAS (Journal of Analytical Atomic Spectrometry) Type: main |
| ResultId | 1 |
