The influence of the metal cations and microhydration on the reaction trajectory of the N3 ↔ O2 thymine proton transfer: Quantum mechanical study

Filip Šebesta, Mateusz Z. Brela, Silvia Diaz, Sebastian Miranda, Jane S. Murray, Soledad Gutiérrez-Oliva, Alejandro Toro-Labbé, Artur Michalak, Jaroslav V. Burda

Resultado de la investigación: Article

2 Citas (Scopus)

Resumen

This study involves the intramolecular proton transfer (PT) process on a thymine nucleobase between N3 and O2 atoms. We explore a mechanism for the PT assisted by hexacoordinated divalent metals cations, namely Mg2+, Zn2+, and Hg2+. Our results point out that this reaction corresponds to a two-stage process. The first involves the PT from one of the aqua ligands toward O2. The implications of this stage are the formation of a hydroxo anion bound to the metal center and a positively charged thymine. To proceed to the second stage, a structural change is needed to allow the negatively charged hydroxo ligand to abstract the N3 proton, which represents the final product of the PT reaction. In the presence of the selected hexaaqua cations, the activation barrier is at most 8 kcal/mol.

Idioma originalEnglish
Páginas (desde-hasta)2680-2692
Número de páginas13
PublicaciónJournal of Computational Chemistry
Volumen38
N.º31
DOI
EstadoPublished - 5 dic 2017

Huella dactilar

Proton transfer
Thymine
Cations
Metals
Positive ions
Trajectories
Trajectory
Ligands
Structural Change
Anions
Protons
Activation
Negative ions
Chemical activation
Atoms
Influence

ASJC Scopus subject areas

  • Chemistry(all)
  • Computational Mathematics

Citar esto

Šebesta, Filip ; Brela, Mateusz Z. ; Diaz, Silvia ; Miranda, Sebastian ; Murray, Jane S. ; Gutiérrez-Oliva, Soledad ; Toro-Labbé, Alejandro ; Michalak, Artur ; Burda, Jaroslav V. / The influence of the metal cations and microhydration on the reaction trajectory of the N3 ↔ O2 thymine proton transfer : Quantum mechanical study. En: Journal of Computational Chemistry. 2017 ; Vol. 38, N.º 31. pp. 2680-2692.
@article{35e0ce7f7a1f402393d981defd7fe37a,
title = "The influence of the metal cations and microhydration on the reaction trajectory of the N3 ↔ O2 thymine proton transfer: Quantum mechanical study",
abstract = "This study involves the intramolecular proton transfer (PT) process on a thymine nucleobase between N3 and O2 atoms. We explore a mechanism for the PT assisted by hexacoordinated divalent metals cations, namely Mg2+, Zn2+, and Hg2+. Our results point out that this reaction corresponds to a two-stage process. The first involves the PT from one of the aqua ligands toward O2. The implications of this stage are the formation of a hydroxo anion bound to the metal center and a positively charged thymine. To proceed to the second stage, a structural change is needed to allow the negatively charged hydroxo ligand to abstract the N3 proton, which represents the final product of the PT reaction. In the presence of the selected hexaaqua cations, the activation barrier is at most 8 kcal/mol.",
keywords = "chemical potential, DFT, proton transfer, reaction coordinate, thymine",
author = "Filip Šebesta and Brela, {Mateusz Z.} and Silvia Diaz and Sebastian Miranda and Murray, {Jane S.} and Soledad Guti{\'e}rrez-Oliva and Alejandro Toro-Labb{\'e} and Artur Michalak and Burda, {Jaroslav V.}",
year = "2017",
month = "12",
day = "5",
doi = "10.1002/jcc.24911",
language = "English",
volume = "38",
pages = "2680--2692",
journal = "Journal of Computational Chemistry",
issn = "0192-8651",
publisher = "John Wiley and Sons Inc.",
number = "31",

}

Šebesta, F, Brela, MZ, Diaz, S, Miranda, S, Murray, JS, Gutiérrez-Oliva, S, Toro-Labbé, A, Michalak, A & Burda, JV 2017, 'The influence of the metal cations and microhydration on the reaction trajectory of the N3 ↔ O2 thymine proton transfer: Quantum mechanical study', Journal of Computational Chemistry, vol. 38, n.º 31, pp. 2680-2692. https://doi.org/10.1002/jcc.24911

The influence of the metal cations and microhydration on the reaction trajectory of the N3 ↔ O2 thymine proton transfer : Quantum mechanical study. / Šebesta, Filip; Brela, Mateusz Z.; Diaz, Silvia; Miranda, Sebastian; Murray, Jane S.; Gutiérrez-Oliva, Soledad; Toro-Labbé, Alejandro; Michalak, Artur; Burda, Jaroslav V.

En: Journal of Computational Chemistry, Vol. 38, N.º 31, 05.12.2017, p. 2680-2692.

Resultado de la investigación: Article

TY - JOUR

T1 - The influence of the metal cations and microhydration on the reaction trajectory of the N3 ↔ O2 thymine proton transfer

T2 - Quantum mechanical study

AU - Šebesta, Filip

AU - Brela, Mateusz Z.

AU - Diaz, Silvia

AU - Miranda, Sebastian

AU - Murray, Jane S.

AU - Gutiérrez-Oliva, Soledad

AU - Toro-Labbé, Alejandro

AU - Michalak, Artur

AU - Burda, Jaroslav V.

PY - 2017/12/5

Y1 - 2017/12/5

N2 - This study involves the intramolecular proton transfer (PT) process on a thymine nucleobase between N3 and O2 atoms. We explore a mechanism for the PT assisted by hexacoordinated divalent metals cations, namely Mg2+, Zn2+, and Hg2+. Our results point out that this reaction corresponds to a two-stage process. The first involves the PT from one of the aqua ligands toward O2. The implications of this stage are the formation of a hydroxo anion bound to the metal center and a positively charged thymine. To proceed to the second stage, a structural change is needed to allow the negatively charged hydroxo ligand to abstract the N3 proton, which represents the final product of the PT reaction. In the presence of the selected hexaaqua cations, the activation barrier is at most 8 kcal/mol.

AB - This study involves the intramolecular proton transfer (PT) process on a thymine nucleobase between N3 and O2 atoms. We explore a mechanism for the PT assisted by hexacoordinated divalent metals cations, namely Mg2+, Zn2+, and Hg2+. Our results point out that this reaction corresponds to a two-stage process. The first involves the PT from one of the aqua ligands toward O2. The implications of this stage are the formation of a hydroxo anion bound to the metal center and a positively charged thymine. To proceed to the second stage, a structural change is needed to allow the negatively charged hydroxo ligand to abstract the N3 proton, which represents the final product of the PT reaction. In the presence of the selected hexaaqua cations, the activation barrier is at most 8 kcal/mol.

KW - chemical potential

KW - DFT

KW - proton transfer

KW - reaction coordinate

KW - thymine

UR - http://www.scopus.com/inward/record.url?scp=85030107400&partnerID=8YFLogxK

U2 - 10.1002/jcc.24911

DO - 10.1002/jcc.24911

M3 - Article

C2 - 28925001

AN - SCOPUS:85030107400

VL - 38

SP - 2680

EP - 2692

JO - Journal of Computational Chemistry

JF - Journal of Computational Chemistry

SN - 0192-8651

IS - 31

ER -