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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...

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Autores principales: 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.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
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.
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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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