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Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides
The complexation of trivalent lanthanides and minor actinides (Am(3+), Cm(3+), and Cf(3+)) by the acyclic aminopolycarboxylate chelators 6,6′-((ethane-1,2-diylbis–((carboxymethyl)azanediyl))bis–(methylene))dipicolinic acid (H(4)octapa) and 6,6'-((((4-(1-(2-(2-(2-hydroxyethoxy)ethoxy)ethyl)-1H-1...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10587169/ https://www.ncbi.nlm.nih.gov/pubmed/37857726 http://dx.doi.org/10.1038/s41598-023-44106-6 |
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author | Pilgrim, Corey D. Grimes, Travis S. Smith, Clayn Heathman, Colt R. Mathew, Jopaul Jansone-Popova, Santa Roy, Santanu Ray, Debmalya Bryantsev, Vyacheslav S. Zalupski, Peter R. |
author_facet | Pilgrim, Corey D. Grimes, Travis S. Smith, Clayn Heathman, Colt R. Mathew, Jopaul Jansone-Popova, Santa Roy, Santanu Ray, Debmalya Bryantsev, Vyacheslav S. Zalupski, Peter R. |
author_sort | Pilgrim, Corey D. |
collection | PubMed |
description | The complexation of trivalent lanthanides and minor actinides (Am(3+), Cm(3+), and Cf(3+)) by the acyclic aminopolycarboxylate chelators 6,6′-((ethane-1,2-diylbis–((carboxymethyl)azanediyl))bis–(methylene))dipicolinic acid (H(4)octapa) and 6,6'-((((4-(1-(2-(2-(2-hydroxyethoxy)ethoxy)ethyl)-1H-1,2,3-triazol-4-yl)pyridine-2,6-diyl)bis–(methylene))bis–((carboxymethyl)azanediyl))bis–(methylene)) dipicolinic acid (H(4)pypa-peg) were studied using potentiometry, spectroscopy, competitive complexation liquid–liquid extraction, and ab initio molecular dynamics simulations. Two studied reagents are strong multidentate chelators, well-suited for applications seeking radiometal coordination for in-vivo delivery and f-element isolation. The previously reported H(4)octapa forms a compact coordination packet, while H(4)pypa-peg is less sterically constrained due to the presence of central pyridine ring. The solubility of H(4)octapa is limited in a non-complexing high ionic strength perchlorate media. However, the introduction of a polyethylene glycol group in H(4)pypa-peg increased the solubility without influencing its ability to complex the lanthanides and minor actinides in solution. |
format | Online Article Text |
id | pubmed-10587169 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-105871692023-10-21 Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides Pilgrim, Corey D. Grimes, Travis S. Smith, Clayn Heathman, Colt R. Mathew, Jopaul Jansone-Popova, Santa Roy, Santanu Ray, Debmalya Bryantsev, Vyacheslav S. Zalupski, Peter R. Sci Rep Article The complexation of trivalent lanthanides and minor actinides (Am(3+), Cm(3+), and Cf(3+)) by the acyclic aminopolycarboxylate chelators 6,6′-((ethane-1,2-diylbis–((carboxymethyl)azanediyl))bis–(methylene))dipicolinic acid (H(4)octapa) and 6,6'-((((4-(1-(2-(2-(2-hydroxyethoxy)ethoxy)ethyl)-1H-1,2,3-triazol-4-yl)pyridine-2,6-diyl)bis–(methylene))bis–((carboxymethyl)azanediyl))bis–(methylene)) dipicolinic acid (H(4)pypa-peg) were studied using potentiometry, spectroscopy, competitive complexation liquid–liquid extraction, and ab initio molecular dynamics simulations. Two studied reagents are strong multidentate chelators, well-suited for applications seeking radiometal coordination for in-vivo delivery and f-element isolation. The previously reported H(4)octapa forms a compact coordination packet, while H(4)pypa-peg is less sterically constrained due to the presence of central pyridine ring. The solubility of H(4)octapa is limited in a non-complexing high ionic strength perchlorate media. However, the introduction of a polyethylene glycol group in H(4)pypa-peg increased the solubility without influencing its ability to complex the lanthanides and minor actinides in solution. Nature Publishing Group UK 2023-10-19 /pmc/articles/PMC10587169/ /pubmed/37857726 http://dx.doi.org/10.1038/s41598-023-44106-6 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Pilgrim, Corey D. Grimes, Travis S. Smith, Clayn Heathman, Colt R. Mathew, Jopaul Jansone-Popova, Santa Roy, Santanu Ray, Debmalya Bryantsev, Vyacheslav S. Zalupski, Peter R. Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides |
title | Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides |
title_full | Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides |
title_fullStr | Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides |
title_full_unstemmed | Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides |
title_short | Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides |
title_sort | tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10587169/ https://www.ncbi.nlm.nih.gov/pubmed/37857726 http://dx.doi.org/10.1038/s41598-023-44106-6 |
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