MSINDO Study of Water Adsorption on the Clean MgO(100) Surface

Tikhomirov, V. A.; Jug, Karl

doi:10.1021/jp9938260

Cited by 20 publications

(14 citation statements)

References 27 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Figure4a,b for regions I and II, respectively, show that the water molecules coordinate together by hydrogen bonding. In region I, this occurs via chains of water molecules, similar to the clustering of water at sub-monolayer coverages previously seen by simulation 61. A disruption of the chain structure is seen in region II, due to the adsorption of water molecules on top of the chain, rather than directly on the surface.Interestingly, it can be seen that merely reducing the partial pressure of water would not result in carbonation.…”

supporting

confidence: 65%

Atomistic Simulation of Surface Selectivity on Carbonate Formation at Calcium and Magnesium Oxide Surfaces

2012

View full text Add to dashboard Cite

We report atom-level simulations of the surface selectivity and the resulting surface phase diagrams for the {100}, {110}, {111}, and {310} surfaces of CaO and MgO as a function of varying CO 2 and H 2 O partial pressures. This work extends the traditional approach based on ab initio calculations, which can be time-consuming and costly for large systems, by using semiempirical atomistic simulations. The advantage of this approach is that very large numbers of calculations can be performed, thereby allowing a more effective search of the configurational space. The resulting free energies are used to generate the surface phase diagrams. The results indicate that the {100} surfaces of MgO and CaO show different dominant phases at atmospheric concentrations of gaseous water and carbon dioxide. The CaO surface forms a carbonated phase, whereas the MgO surface contains associatively adsorbed water. On the other hand, both {111} surfaces show the dominance of surface hydroxylation, effectively forming a layer of mineral hydroxide, with carbonation only observed at very high carbon dioxide concentrations. Finally, the {310} surfaces show enhanced reactivity with carbonate, most likely a result of the steps on the surfaces. In general, we predict that the minimum CO 2 partial pressure needed to carbonate these surfaces can be controlled by the water partial pressure. The effect of temperature is also considered, and the results show how the number of surface adsorbates decreases as temperature increases.

show abstract

supporting

confidence: 65%

Atomistic Simulation of Surface Selectivity on Carbonate Formation at Calcium and Magnesium Oxide Surfaces

2012

View full text Add to dashboard Cite

show abstract

“…There is good agreement of the calculated dimerization energy with the experimental value. The suitability of the method for solid state simulation and adsorption studies also for third-row elements has been documented [24,[37][38][39][40][41][42][43][44][45]. Differently from our earlier studies on MgO, where we had used the free or embedded cluster models for surface simulations, our present calculations are based on the cyclic cluster model for ionic systems [46] including long electrostatic range effects (CCMM) [47].…”

Section: Computational Detailsmentioning

confidence: 99%

Cyclic cluster study of water adsorption structures on the MgO(100) surface

Jug¹,

Heidberg²,

Bredow³

2007

Surface Science

Self Cite

View full text Add to dashboard Cite

“…The nature of water adsorption on the MgO(100) surface has attracted considerable attention, being the subject of several experimental and theoretical studies. [1][2][3][4][5][6][7][8][9] It appears that even at low coverages, molecularly adsorbed water is H-bonded to surface OH groups resulting from water dissociation and, as a result, an experimental value for the interaction energy of an isolated water molecule with the surface is not available. On the computational side, the water/ MgO system has been investigated using semi-empirical methods, 8 density functional theory (DFT), 1 and a mixed Hartree-Fock/coupled-cluster procedure combined with an embedded cluster model.…”

Section: Introductionmentioning

confidence: 99%

Adsorption of a water molecule on the MgO(100) surface as described by cluster and slab models

Karalti

Gillan

Jordan

2012

Phys. Chem. Chem. Phys.

View full text Add to dashboard Cite

The interaction of a water molecule with the (100) surface of MgO as described by cluster models is studied using MP2, coupled MP2 (MP2C) and symmetry-adapted perturbation theory (SAPT) methods. In addition, diffusion Monte Carlo (DMC) results are presented for several slab models as well as for the smallest, 2X2 cluster model. For the 2X2 model it is found that the MP2C, DMC, and CCSD(T) methods give nearly the same potential energy curve for the water-cluster interaction, whereas the potential energy curve from the SAPT calculations differs slightly from those of the other methods. The interaction of the water molecule with the cluster models of the MgO(100) surface is weakened upon expanding the number of layers from one to two and also upon expanding the description of the layers from 2X2 to 4X4 to 6X6. The SAPT calculations reveal that both these expansions of the cluster model are accompanied by reductions in the magnitudes of the induction and dispersion constributions. The best estimate of the energy for binding an isolated water molecule to the surface obtained from the cluster model calculations is in good agreement with that obtained from the DMC calculations using a 2-layer slab model with periodic boundary conditions.

show abstract

MSINDO Study of Water Adsorption on the Clean MgO(100) Surface

Cited by 20 publications

References 27 publications

Atomistic Simulation of Surface Selectivity on Carbonate Formation at Calcium and Magnesium Oxide Surfaces

Atomistic Simulation of Surface Selectivity on Carbonate Formation at Calcium and Magnesium Oxide Surfaces

Cyclic cluster study of water adsorption structures on the MgO(100) surface

Adsorption of a water molecule on the MgO(100) surface as described by cluster and slab models

Contact Info

Product

Resources

About