Publication: Stability of Hydrogen Hydrates from Second-Order Møller-Plesset Perturbation Theory
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Issued Date
2018
Resource Type
File Type
application/pdf
ISSN
19487185
Other identifier(s)
2-s2.0-85053675666
Rights Holder(s)
Scopus
Bibliographic Citation
Journal of Physical Chemistry Letters. Vol 9, No.18 (2018), p.5624-5629
Suggested Citation
Košata J., Merkl P., Teeratchanan P., Hermann A. Stability of Hydrogen Hydrates from Second-Order Møller-Plesset Perturbation Theory. Journal of Physical Chemistry Letters. Vol 9, No.18 (2018), p.5624-5629. doi:10.1021/acs.jpclett.8b02274 Retrieved from: https://hdl.handle.net/20.500.14740/5843
Author(s)
Abstract
The formation of gas hydrates and clathrates critically depends on the interaction between the host water network and the guest gas species. Density functional calculations can struggle to quantitatively capture these dispersion-type interactions. Here, we report wave function-based calculations on hydrogen hydrates that combine periodic Hartree-Fock with a localized treatment of electronic correlation. We show that local second-order Møller-Plesset perturbation theory (LMP2) reproduces the stability of the different filled-ice-like hydrates in excellent agreement with experimental data. In contrast to various dispersion-corrected density functional theory implementations, LMP2 correctly identifies the pressures needed to stabilize the C0, C1, and C2 hydrates and does not find a spurious region of stability for an ice-Ih-based dihydrate. Our results suggest that LMP2 or similar approaches can provide quantitative insights into the mechanisms of formation and eventual decomposition of molecular host-guest compounds. © 2018 American Chemical Society.
Subject(s)
Density of gases
Dispersion (waves)
Gas hydrates
Hydration
Hydrogen
Perturbation techniques
Wave functions
Dispersion-corrected density functional
Electronic correlation
Host-guest compound
Localized treatment
Mechanisms of formation
Periodic Hartree-Fock
Plesset perturbation theory
Region of stabilities
Density functional theory
Article
Decomposition
Density functional theory
Hydration
Quantitative analysis
Dispersion (waves)
Gas hydrates
Hydration
Hydrogen
Perturbation techniques
Wave functions
Dispersion-corrected density functional
Electronic correlation
Host-guest compound
Localized treatment
Mechanisms of formation
Periodic Hartree-Fock
Plesset perturbation theory
Region of stabilities
Density functional theory
Article
Decomposition
Density functional theory
Hydration
Quantitative analysis