Quantum effects and anharmonicity in the H2-Li(+)-benzene complex: a model for hydrogen storage materials

The Journal of Chemical Physics
Stephen J KolmannMeredith J T Jordan

Abstract

Quantum and anharmonic effects are investigated in H2-Li(+)-benzene, a model for hydrogen adsorption in metal-organic frameworks and carbon-based materials. Three- and 8-dimensional quantum diffusion Monte Carlo (QDMC) and rigid-body diffusion Monte Carlo (RBDMC) simulations are performed on potential energy surfaces interpolated from electronic structure calculations at the M05-2X/6-31+G(d,p) and M05-2X/6-311+G(2df,p) levels of theory using a three-dimensional spline or a modified Shepard interpolation. These calculations investigate the intermolecular interactions in this system, with three- and 8-dimensional 0 K H2 binding enthalpy estimates, ΔH(bind) (0 K), being 16.5 kJ mol(-1) and 12.4 kJ mol(-1), respectively: 0.1 and 0.6 kJ mol(-1) higher than harmonic values. Zero-point energy effects are 35% of the value of ΔH(bind) (0 K) at M05-2X/6-311+G(2df,p) and cannot be neglected; uncorrected electronic binding energies overestimate ΔHbind (0 K) by at least 6 kJ mol(-1). Harmonic intermolecular binding enthalpies can be corrected by treating the H2 "helicopter" and "ferris wheel" rotations as free and hindered rotations, respectively. These simple corrections yield results within 2% of the 8-dimensional anharmonic calculations....Continue Reading

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Citations

Sep 1, 2015·The Journal of Physical Chemistry. a·Jordan H D'ArcyMichael A Collins
Nov 23, 2015·The Journal of Chemical Physics·Lachlan P LindoyMeredith J T Jordan
Aug 25, 2015·The Journal of Chemical Physics·Jordan H D'ArcyMeredith J T Jordan
Sep 2, 2015·Physical Chemistry Chemical Physics : PCCP·Martin PykalMichal Otyepka

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Methods Mentioned

BETA
inelastic neutron scattering

Software Mentioned

Grow
Gaussian03

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