@article{10272/17596,
year = {2017},
url = {http://hdl.handle.net/10272/17596},
abstract = {Carbon dioxide (CO2) molecules show a rich orientation landscape when they are enclathrated in type I hydrates. Previous studies have described experimentally their preferential orientations, and some theoretical works have explained, but only partially, these experimental results. In the present paper, we use classical molecular dynamics and electronic density functional theory to advance in the theoretical description of CO2 orientations within type I hydrates. Our results are fully compatible with those previously reported, both theoretical and experimental, the geometric shape of the cavities in hydrate being, and therefore, the steric constraints, responsible for some (but not all) preferential angles. In addition, our calculations also show that guest–guest interactions in neighbouring cages are a key factor to explain the remaining experimental angles. Besides the implication concerning equation of state hydrate modeling approximations, the conclusion is that these guest–guest interactions should not be neglected, contrary to the usual practice.},
organization = {The authors acknowledge Centro de Supercomputación de Galicia (CESGA, Santiago de Compostela, Spain) for providing access to computing facilities, and Ministerio de Economía y Competitividad (MINECO, Spain) for financial support (FIS2013- 46920-C2-1-P and FIS2015-68910-P). The authors also acknowledge MCIA (Mésocentre de Calcul Intensif Aquitain) of the Universités de Bordeaux and Pau et Pays de l’Adour, France, for the computer resources provided for this work (JMM) and Carnot Institute ISIFoR (France) through the THEMYS project (JMM, JPT).},
publisher = {Royal Society of Chemistry},
title = {Computational study of the interplay between intermolecular interactions and CO2 orientations in type I hydrates},
author = {Pérez Rodríguez, Martín and Vidal Vidal, Ángel and Míguez Díaz, José Manuel and Jiménez Blas, Felipe and Torré, Jean-Philippe},
}