6533b82bfe1ef96bd128e1e1
RESEARCH PRODUCT
A Grand Canonical Monte Carlo Study of the N2, CO, and Mixed N2–CO Clathrate Hydrates
J. Marcos SalazarJean-marc SimonSylvain PicaudAntoine Pattsubject
Materials scienceClathrate hydrateThermodynamics02 engineering and technologyTrappingAtmospheric temperature range010402 general chemistry021001 nanoscience & nanotechnology01 natural sciences0104 chemical sciencesSurfaces Coatings and FilmsElectronic Optical and Magnetic MaterialsGas phase[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistryGeneral EnergyAdsorptionMoleculeFugacityPhysical and Theoretical Chemistry[PHYS.ASTR]Physics [physics]/Astrophysics [astro-ph]0210 nano-technologyComputingMilieux_MISCELLANEOUSGrand canonical monte carlodescription
In this paper we report the use of Grand Canonical Monte Carlo (GCMC) simulations to characterize the competitive trapping of CO and N2 molecules into clathrates, for various gas compositions in the temperature range from 50 to 150 K. The simulations evidence a preferential trapping of CO with respect to N2. This leads to the formation of clathrates that are preferentially filled with CO at equilibrium, irrespective of the composition of the gas phase, the fugacity, and the temperature. Moreover, the results of the simulations show that the small cages of the clathrate structure are always filled first, independent of either the guest structure or the temperature. This issue has been associated with the rather significant differences in the calculated heats of encapsulation (∼2–3 kJ/mol) between the smallest and the largest cages. In addition, calculations with the simplified ideal adsorbed solution theory (IAST) are developed to allow a comparison with the results arising from the GCMC simulations. Inter...
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2018-07-18 | The Journal of Physical Chemistry C |