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Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density

The interaction natures between Pu and different ligands in several plutonyl (VI) complexes are investigated by performing topological analyses of electron density. The geometrical structures in both gaseous and aqueous phases are obtained with B3LYP functional, and are generally in agreement with a...

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Autores principales: Du, Jiguang, Sun, Xiyuan, Jiang, Gang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2016
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4848887/
https://www.ncbi.nlm.nih.gov/pubmed/27077844
http://dx.doi.org/10.3390/ijms17040414
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author Du, Jiguang
Sun, Xiyuan
Jiang, Gang
author_facet Du, Jiguang
Sun, Xiyuan
Jiang, Gang
author_sort Du, Jiguang
collection PubMed
description The interaction natures between Pu and different ligands in several plutonyl (VI) complexes are investigated by performing topological analyses of electron density. The geometrical structures in both gaseous and aqueous phases are obtained with B3LYP functional, and are generally in agreement with available theoretical and experimental results when combined with all-electron segmented all-electron relativistic contracted (SARC) basis set. The Pu– [Formula: see text] bond orders show significant linear dependence on bond length and the charge of oxygen atoms in plutonyl moiety. The closed-shell interactions were identified for Pu-Ligand bonds in most complexes with quantum theory of atoms in molecules (QTAIM) analyses. Meanwhile, we found that some Pu–Ligand bonds, like Pu–OH(−), show weak covalent. The interactive nature of Pu–ligand bonds were revealed based on the interaction quantum atom (IQA) energy decomposition approach, and our results indicate that all Pu–Ligand interactions is dominated by the electrostatic attraction interaction as expected. Meanwhile it is also important to note that the quantum mechanical exchange-correlation contributions can not be ignored. By means of the non-covalent interaction (NCI) approach it has been found that some weak and repulsion interactions existed in plutonyl(VI) complexes, which can not be distinguished by QTAIM, can be successfully identified.
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spelling pubmed-48488872016-05-04 Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density Du, Jiguang Sun, Xiyuan Jiang, Gang Int J Mol Sci Article The interaction natures between Pu and different ligands in several plutonyl (VI) complexes are investigated by performing topological analyses of electron density. The geometrical structures in both gaseous and aqueous phases are obtained with B3LYP functional, and are generally in agreement with available theoretical and experimental results when combined with all-electron segmented all-electron relativistic contracted (SARC) basis set. The Pu– [Formula: see text] bond orders show significant linear dependence on bond length and the charge of oxygen atoms in plutonyl moiety. The closed-shell interactions were identified for Pu-Ligand bonds in most complexes with quantum theory of atoms in molecules (QTAIM) analyses. Meanwhile, we found that some Pu–Ligand bonds, like Pu–OH(−), show weak covalent. The interactive nature of Pu–ligand bonds were revealed based on the interaction quantum atom (IQA) energy decomposition approach, and our results indicate that all Pu–Ligand interactions is dominated by the electrostatic attraction interaction as expected. Meanwhile it is also important to note that the quantum mechanical exchange-correlation contributions can not be ignored. By means of the non-covalent interaction (NCI) approach it has been found that some weak and repulsion interactions existed in plutonyl(VI) complexes, which can not be distinguished by QTAIM, can be successfully identified. MDPI 2016-04-11 /pmc/articles/PMC4848887/ /pubmed/27077844 http://dx.doi.org/10.3390/ijms17040414 Text en © 2016 by the authors; licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons by Attribution (CC-BY) license (http://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Du, Jiguang
Sun, Xiyuan
Jiang, Gang
Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density
title Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density
title_full Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density
title_fullStr Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density
title_full_unstemmed Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density
title_short Exploring the Interaction Natures in Plutonyl (VI) Complexes with Topological Analyses of Electron Density
title_sort exploring the interaction natures in plutonyl (vi) complexes with topological analyses of electron density
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4848887/
https://www.ncbi.nlm.nih.gov/pubmed/27077844
http://dx.doi.org/10.3390/ijms17040414
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