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Theoretical Study of Actinide(III)-DOTA Complexes
[Image: see text] 1,4,7,10-Tetraazacyclododecane-N,N′,N″,N‴-tetraacetic acid (DOTA) is a prominent chelating ligand used in imaging contrast agents and radiopharmaceuticals. The present study explores the stabilities, structures, and bonding properties of its complexes with trivalent actinides (Ac,...
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Formato: | Online Artículo Texto |
Lenguaje: | English |
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American Chemical Society
2021
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8158830/ https://www.ncbi.nlm.nih.gov/pubmed/34056480 http://dx.doi.org/10.1021/acsomega.1c01292 |
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author | Kovács, Attila |
author_facet | Kovács, Attila |
author_sort | Kovács, Attila |
collection | PubMed |
description | [Image: see text] 1,4,7,10-Tetraazacyclododecane-N,N′,N″,N‴-tetraacetic acid (DOTA) is a prominent chelating ligand used in imaging contrast agents and radiopharmaceuticals. The present study explores the stabilities, structures, and bonding properties of its complexes with trivalent actinides (Ac, U, Np, Pu, Am, Cm, Cf) using density functional theory and relativistic multireference calculations. For reference purposes, the La- and Lu-DOTA complexes are also included. Similar to La(3+), the large An(3+) ions prefer the TSAP conformer of the ligand. The An–ligand bonding is mainly electrostatic, with minor charge transfer contributions to the An 6d orbitals. For the assessment of the thermodynamic stabilities in aqueous solution, PCM radii to use in conjunction with the SMD solvation model were developed. Basically, the thermodynamic stability of the DOTA complexes increases along the An row but with notable counteracting of spin–orbit coupling. |
format | Online Article Text |
id | pubmed-8158830 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-81588302021-05-28 Theoretical Study of Actinide(III)-DOTA Complexes Kovács, Attila ACS Omega [Image: see text] 1,4,7,10-Tetraazacyclododecane-N,N′,N″,N‴-tetraacetic acid (DOTA) is a prominent chelating ligand used in imaging contrast agents and radiopharmaceuticals. The present study explores the stabilities, structures, and bonding properties of its complexes with trivalent actinides (Ac, U, Np, Pu, Am, Cm, Cf) using density functional theory and relativistic multireference calculations. For reference purposes, the La- and Lu-DOTA complexes are also included. Similar to La(3+), the large An(3+) ions prefer the TSAP conformer of the ligand. The An–ligand bonding is mainly electrostatic, with minor charge transfer contributions to the An 6d orbitals. For the assessment of the thermodynamic stabilities in aqueous solution, PCM radii to use in conjunction with the SMD solvation model were developed. Basically, the thermodynamic stability of the DOTA complexes increases along the An row but with notable counteracting of spin–orbit coupling. American Chemical Society 2021-05-11 /pmc/articles/PMC8158830/ /pubmed/34056480 http://dx.doi.org/10.1021/acsomega.1c01292 Text en © 2021 The Author. Published by American Chemical Society Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/). |
spellingShingle | Kovács, Attila Theoretical Study of Actinide(III)-DOTA Complexes |
title | Theoretical Study of Actinide(III)-DOTA Complexes |
title_full | Theoretical Study of Actinide(III)-DOTA Complexes |
title_fullStr | Theoretical Study of Actinide(III)-DOTA Complexes |
title_full_unstemmed | Theoretical Study of Actinide(III)-DOTA Complexes |
title_short | Theoretical Study of Actinide(III)-DOTA Complexes |
title_sort | theoretical study of actinide(iii)-dota complexes |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8158830/ https://www.ncbi.nlm.nih.gov/pubmed/34056480 http://dx.doi.org/10.1021/acsomega.1c01292 |
work_keys_str_mv | AT kovacsattila theoreticalstudyofactinideiiidotacomplexes |