Charge distribution in metal organic framework materials: transferability to a preliminary molecular simulation study of the CO2 adsorption in the MIL-53 (Al) system

Literature Information

Publication Date 2006-11-15
DOI 10.1039/B613378A
Impact Factor 3.676
Authors

N. A. Ramsahye, G. Maurin, S. Bourrelly, P. Llewellyn, T Loiseau, G. Ferey


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Abstract

Density functional theory calculations have been performed in order to extract the charge distribution in the aluminium-containing MIL-53 structure, to allow further computational studies of adsorption in these materials. Both cluster and periodic methods have been used and the charges calculated for each atom constituting the organic and inorganic part of the material, were discussed. Preliminary grand canonical Monte Carlo simulations, based on a consistent set of potential parameters and this newly derived charge distribution, predicted for enthalpies of adsorption for CO2 at low coverage in the “large” and “narrow” pore versions of MIL-53 (Al) to be significantly different. These calculated enthalpies reproduced the two distinct ranges of values observed by microcalorimetry on either side of 6 bars quite well. This agreement between experiment and simulation validated our previous assumption, suggesting a structural switching of the hybrid material during the adsorption process. The microscopic mode of interaction between the hybrid porous framework and the CO2 adsorption was then carefully analysed in both of the MIL-53 (Al) structures.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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