Dynamics of water molecules and sodium ions in solid hydrates of nucleotides

0430610 - ÚOCHB 2015 RIV GB eng J - Článek v odborném periodiku
Dračínský, Martin - Šála, Michal - Hodgkinson, P.
Dynamics of water molecules and sodium ions in solid hydrates of nucleotides.
CrystEngComm. Roč. 16, č. 29 (2014), s. 6756-6764. ISSN 1466-8033
Grant CEP: GA ČR GA13-24880S
Grant ostatní: Seventh Framework Programme of the European Union(XE) FP7-299242 People
Program: FP7
Institucionální podpora: RVO:61388963
Klíčová slova: molecular dynamics simulations * NMR spectroscopy * DFT calculations
Kód oboru RIV: CC - Organická chemie
Impakt faktor: 4.034, rok: 2014

Nuclear magnetic resonance experiments, together with molecular dynamics simulations and NMR calculations, are used to investigate mobility of water molecules and sodium ions in solid hydrates of two nucleotides. The structure of guanosine monophosphate system (GMP) is relatively rigid, with a well-ordered solvation shell of the nucleotide, while the water molecules in the uridine monophosphate system (UMP) are shown to be remarkably mobile, even at -80 degrees C. The disorder of water molecules is observed in the C-13, P-31, and Na-23 solid-state NMR experiments as multiple signals for equivalent sites of the nucleotide corresponding to different local arrangements of the solvation shell. Deuterium NMR spectra of the samples recrystallized from D2O also confirm differences in water mobility between the two systems. The experiments were complemented with NMR calculations on an ensemble of structures obtained from DFT molecular dynamics (MD) simulations. The MD simulations confirmed higher water mobility in the UMP system and the calculated chemical shifts and quadrupolar couplings were consistent with the experimental data. The disordered solvation shell in UMP is likely to be a good model for solvated nucleotides in general, with fast reorientation of water molecules and fluctuations in the hydrogen-bond network.
Trvalý link: http://hdl.handle.net/11104/0235573