Molecular hydrogen solvated in water – A computational study
- Department of Physical Chemistry, Chemical Faculty, Gdańsk University of Technology, Narutowicza 11/12, 80-233 Gdańsk (Poland)
The aqueous hydrogen molecule is studied with molecular dynamics simulations at ambient temperature and pressure conditions, using a newly developed flexible and polarizable H{sub 2} molecule model. The design and implementation of this model, compatible with an existing flexible and polarizable force field for water, is presented in detail. The structure of the hydration layer suggests that first-shell water molecules accommodate the H{sub 2} molecule without major structural distortions and two-dimensional, radial-angular distribution functions indicate that as opposed to strictly tangential, the orientation of these water molecules is such that the solute is solvated with one of the free electron pairs of H{sub 2}O. The calculated self-diffusion coefficient of H{sub 2}(aq) agrees very well with experimental results and the time dependence of mean square displacement suggests the presence of caging on a time scale corresponding to hydrogen bond network vibrations in liquid water. Orientational correlation function of H{sub 2} experiences an extremely short-scale decay, making the H{sub 2}–H{sub 2}O interaction potential essentially isotropic by virtue of rotational averaging. The inclusion of explicit polarizability in the model allows for the calculation of Raman spectra that agree very well with available experimental data on H{sub 2}(aq) under differing pressure conditions, including accurate reproduction of the experimentally noted trends with solute pressure or concentration.
- OSTI ID:
- 22493421
- Journal Information:
- Journal of Chemical Physics, Vol. 143, Issue 24; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
Similar Records
Tracking structural solvent reorganization and recombination dynamics following e– photoabstraction from aqueous I– with femtosecond x-ray spectroscopy and scattering
Computation of methodology-independent single-ion solvation properties from molecular simulations. IV. Optimized Lennard-Jones interaction parameter sets for the alkali and halide ions in water
Related Subjects
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
AMBIENT TEMPERATURE
ANGULAR DISTRIBUTION
COMPUTERIZED SIMULATION
CONCENTRATION RATIO
CORRELATION FUNCTIONS
ELECTRON PAIRS
HYDRATION
HYDROGEN
LAYERS
LIQUIDS
MOLECULAR DYNAMICS METHOD
MOLECULES
POLARIZABILITY
POTENTIALS
RAMAN SPECTRA
SELF-DIFFUSION
SOLUTES
TIME DEPENDENCE
TWO-DIMENSIONAL SYSTEMS
WATER