Ion–water cluster free energy computer simulation using some of most popular ion–water and water–water pair interaction models

Lukyanov, Sergey I.; Zidi, Z.S.; Шевкунов, С. В.

doi:10.1016/j.chemphys.2006.11.022

Cited by 51 publications

(16 citation statements)

References 51 publications

(94 reference statements)

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“…for alkali cation and halogen anion water clusters for n=1 to 6 (Table 3 in that publication). 15 The experimental free energy values for each of the eight alkali or halogen ions decrease irregularly with cluster size, but are generally reduced by about 30% per additional water. This decrease in cluster affinity with cluster size reduces the mean cluster size from that given by equation (2).…”

Section: Resultsmentioning

confidence: 98%

Control of Chemical Effects in the Separation Process of a Differential Mobility Mass Spectrometer System

Schneider¹,

Covey²,

Coy

et al. 2010

Eur J Mass Spectrom (Chichester)

100

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Differential mobility spectrometry (DMS) separates ions on the basis of the difference in their migration rates under high versus low electric fields. Several models describing the physical nature of this field mobility dependence have been proposed but emerging as a dominant effect is the clusterization model sometimes referred to as the dynamic cluster-decluster model. DMS resolution and peak capacity is strongly influenced by the addition of modifiers which results in the formation and dissociation of clusters. This process increases selectivity due to the unique chemical interactions that occur between an ion and neutral gas phase molecules. It is thus imperative to bring the parameters influencing the chemical interactions under control and find ways to exploit them in order to improve the analytical utility of the device. In this paper we describe three important areas that need consideration in order to stabilize and capitalize on the chemical processes that dominate a DMS separation. The first involves means of controlling the dynamic equilibrium of the clustering reactions with high concentrations of specific reagents. The second area involves a means to deal with the unwanted heterogeneous cluster ion populations emitted from the electrospray ionization process that degrade resolution and sensitivity. The third involves fine control of parameters that affect the fundamental collision processes, temperature and pressure.

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Section: Resultsmentioning

confidence: 98%

Control of Chemical Effects in the Separation Process of a Differential Mobility Mass Spectrometer System

Schneider¹,

Covey²,

Coy

et al. 2010

Eur J Mass Spectrom (Chichester)

100

View full text Add to dashboard Cite

show abstract

“…Likewise, Lamoureux and Roux adjusted the ion-water parameters based on their SWM4-DP model of water to reproduce the empirical enthalpies of ion monohydrates and found that the resulting model was able to predict reasonably well selected ab initio energies of larger clusters [21]. Shevkunov used experimental cluster-ion thermodynamic properties to design a non-polarizable force field specifically for the description of Cl À water clusters [130], while Lukyanov et al performed an extensive systematic evaluation of the capability of a set of simple polarizable and non-polarizable models to predict cluster-ion binding hydration Gibbs free energies, enthalpies and entropies [48]. The analysis has been recently extended by Zidi using a fluctuating charge polarizable model [131].…”

Section: Small Cluster Ionsmentioning

confidence: 98%

“…To overcome the size and time limitations of current quantum mechanical methods, classical simulations with quantum-mechanically and empirically derived force fields may serve as a reasonable approximation [21,[48][49][50][51][52]. At the same time, small cluster ion systems with their strong electric fields and large anisotropy of molecular interactions present a significant challenge for effective classical molecular models and can therefore serve as a benchmark for development and evaluation of such models.…”

Section: Small Cluster Ionsmentioning

confidence: 99%

“…The experimental results have been used as anchoring points for the extrapolation of hydration properties to bulk conditions [7,29], as well as for the development and validation of classical molecular force fields [21,[48][49][50][51][52]. The small size of cluster ions, comprising typically less than 10 water molecules, also provides a more direct insight into the specific details of ion-water interactions than that in bulk aqueous systems, which makes these systems a valuable source of information for force field optimization.…”

Section: Cluster Ionsmentioning

confidence: 99%

See 1 more Smart Citation

Single-ion hydration thermodynamics from clusters to bulk solutions: Recent insights from molecular modeling

Vlček

Chialvo

2016

Fluid Phase Equilibria

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A B S T R A C TThe importance of single-ion hydration thermodynamic properties for understanding the driving forces of aqueous electrolyte processes, along with the impossibility of their direct experimental measurement, have prompted a large number of experimental, theoretical, and computational studies aimed at separating the cation and anion contributions. Here we provide an overview of historical approaches based on extrathermodynamic assumptions and more recent computational studies of single-ion hydration in order to evaluate the approximations involved in these methods, quantify their accuracy, reliability, and limitations in the light of the latest developments. We also offer new insights into the factors that influence the accuracy of ion-water interaction models and our views on possible ways to fill this substantial knowledge gap in aqueous physical chemistry.

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“…Ion molecular clusters are sites of atmospheric moisture nucleation; however, calculations show that single ions [18][19][20][21][22][23][24][25] and ion pairs [26][27][28][29] cannot stimulate the transition from clustering to avalanche like growth of macroscopic droplets and condensa tion. Larger nucleation centers, the role of which is played by aerosol particles, are necessary to eliminate the free energy barrier, which hinders the droplet growth [30][31][32][33][34][35][36][37][38][39][40][41][42][43][44][45].…”

Section: Introductionmentioning

confidence: 99%

Water vapor clustering in the field of a chlorine anion occurring in a planar nanopore with structureless walls

Шевкунов

2014

Colloid J

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The Monte Carlo bicanonical statistical ensemble method has been employed to calculate the free energy, entropy, and work of Clion hydration in model planar pores 0.5 and 0.7 nm wide at 298 and 400 K. A detailed model of many body interactions with the ion has been used, the model being matched to exper imental data with respect to the free energy and enthalpy of attachment reaction in water vapor. Under the conditions of a restricted volume, the equilibrium size of a hydration shell substantially decreases, with the effect becoming stronger in the range of moderate and large sizes. In moderately supersaturated vapors, under the conditions of a nanopore, the ion loses its hydration shell as the temperature is decreased. In supersatu rated vapors, the hydration shell formed on the ion is thermodynamically stable, while the stability crisis shifts to the region of larger sizes. The enhancement of the thermodynamic stability in the pore results from a rise in the chemical potential of molecules due to the deficiency of closet neighbors and a reduction in the entropy under the conditions of the restricted volume. As the temperature is elevated, the effect of ion displacement out of its hydration shell is leveled. The regularities derived in terms of the estimation model based on the cap illary approximation are in qualitative agreement with the results of computer simulation.

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Ion–water cluster free energy computer simulation using some of most popular ion–water and water–water pair interaction models

Cited by 51 publications

References 51 publications

Control of Chemical Effects in the Separation Process of a Differential Mobility Mass Spectrometer System

Control of Chemical Effects in the Separation Process of a Differential Mobility Mass Spectrometer System

Single-ion hydration thermodynamics from clusters to bulk solutions: Recent insights from molecular modeling

Water vapor clustering in the field of a chlorine anion occurring in a planar nanopore with structureless walls

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