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Formation and interaction of hydrated alkali metal ions at the graphite-water interface

Sheng Meng (Institutionen för teknisk fysik, Material- och ytteori) ; Shiwu Gao
JOURNAL OF CHEMICAL PHYSICS Vol. 125 (2006), (1), p. 014708.
[Artikel, refereegranskad vetenskaplig]

Ion hydration at a solid surface ubiquitously exists in nature and plays important roles in many natural processes and technological applications. Aiming at obtaining a microscopic insight into the formation of such systems and interactions therein, we have investigated the hydration of alkali metal ions at a prototype surface-graphite (0001), using first-principles molecular dynamics simulations. At low water coverage, the alkali metal ions form two-dimensional hydration shells accommodating at most four (Li, Na) and three (K, Rb, Cs) waters in the first shell. These two-dimensional shells generally evolve into three-dimensional structures at higher water coverage, due to the competition between hydration and ion-surface interactions. Exceptionally K was found to reside at the graphite-water interface for water coverages up to bulk water limit, where it forms an "umbrellalike" surface hydration shell with an average water-ion-surface angle of 115 degrees. Interactions between the hydrated K and Na ions at the interface have also been studied. Water molecules seem to mediate an effective ion-ion interaction, which favors the aggregation of Na ions but prevents nucleation of K. These results agree with experimental observations in electron energy loss spectroscopy, desorption spectroscopy, and work function measurement. In addition, the sensitive dependence of charge transfer on dynamical structure evolution during the hydration process, implies the necessity to describe surface ion hydration from electronic structure calculations.

Nyckelord: GENERALIZED GRADIENT APPROXIMATION; DENSITY-FUNCTIONAL THEORY; MOLECULAR-DYNAMICS; AQUEOUS-SOLUTIONS; LIQUID WATER; ADSORPTION; POTASSIUM; SURFACES; H2O; COADSORPTION



Denna post skapades 2007-10-29. Senast ändrad 2010-01-26.
CPL Pubid: 58990

 

Institutioner (Chalmers)

Institutionen för teknisk fysik, Material- och ytteori (1900-2015)
Institutionen för fysik (GU) (GU)

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Ytor och mellanytor
Elektronstruktur
Struktur- och vibrationsfysik
Beräkningsfysik

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