Kinetics of Multicomponent Nanosize Clusters on Solid Surfaces

Brunelli, David N.; Skodje, Rex T.

doi:10.1021/la034435m

Cited by 2 publications

(3 citation statements)

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“…At equilibrium with a single cluster (N,x), the density is uniform in keeping with Fick's law, J i ϭϪDٌ i ϭ0. In a previous report, 27 we have shown that the equilibrium partial pressures surrounding a binary cluster are remarkably well described by a generalization of the Gibbs-Thomson formula,…”

Section: A Rate Constant Expressionsmentioning

confidence: 79%

“…͑2.7͒, either the evaporation or capture rates may be specified, thereby giving both sets of rates. In previous work, 27 we have undertaken large-scale numerical simulations of the evaporation rates that were found to be well represented using fairly simple expressions. Numerical Monte Carlo simulations 19,31,32 on model unary systems indicated that the scaling of the evaporation rates with cluster size shows a very noticeable deviation from the naive expectation, R i e (N,x A )ϰ2r, even for clusters Nϳ100 000.…”

Section: ͑25͒mentioning

confidence: 99%

“…In a previous work, we have considered the properties of single clusters in contact with a multicomponent two-dimensional background gas. 27 Here, we model a collection of interacting clusters representing the binary thin film. The rate-equation formalism of Venables 28 is extended to multicomponent systems.…”

Section: Introductionmentioning

confidence: 99%

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Coarsening of multicomponent thin films

Brunelli

Skodje

2004

Phys. Rev. B

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The theory for the kinetics of coarsening of multicomponent thin films is studied. The growth and decay rates of surface clusters consisting of more than one chemically distinct species are represented through a formalism based on the theory of real solutions. Explicit expressions are presented for the time evolution of a thin film in terms of the quasichemical rate equation approach that describes the concentrations of clusters of variable size and composition. The continuum limit of the rate equations yields a partial differential equation that applies to the late stage growth. It is found that the traditional Lifshitz-Slezov-Wagner approach, which employs a first-order continuity-type equation, is inadequate to treat the compositional variation of the clusters. Instead, a second-order generalized diffusion equation should be used. A model problem of a binary film, consisting of two types of atoms interacting through nearest-neighbor and next-nearest-neighbor coupling, is studied using a dynamical Monte Carlo method. The cluster size and composition distributions are extracted from the simulations as functions of time. The film kinetics exhibits a crossover behavior between coalescencediffusion coarsening at short times and Ostwald ripening at long times. Except for very small cluster sizes, the distributions are well represented by a separable two-dimensional scaling-type solution.

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Section: A Rate Constant Expressionsmentioning

confidence: 79%

Section: ͑25͒mentioning

confidence: 99%

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Coarsening of multicomponent thin films

Brunelli

Skodje

2004

Phys. Rev. B

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Pore Characteristics of Hydrate-Bearing Sediments from Krishna-Godavari Basin, Offshore India

Guan,

Yang,

et al. 2024

JMSE

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Pore-filling hydrates are the main occurrence forms of marine gas hydrates. Pore characteristics are a vital factor affecting the thermodynamic properties of hydrates and their distribution in sediments. Currently, the characterization of the pore system for hydrate-bearing reservoirs are little reported. Therefore, this paper focuses on the Krishna-Godavari Basin, via various methods to characterize the hydrate-bearing sediments in the region. The results showed that X-ray diffraction (XRD) combined with scanning electron microscopy (SEM) and cast thin section (CTS) can better characterize the mineral composition in the reservoir, high-pressure mercury injection (HPMI) focused on the contribution of pore size to permeability, constant-rate mercury injection (CRMI) had the advantage of distinguishing between the pore space and pore throat, and nuclear magnetic resonance cryoporometry (NMRC) technique can not only obtain the pore size distribution of nanopores with a characterization range greater than nitrogen gas adsorption (N2GA), but also quantitatively describe the trend of fluids in the pore system with temperature. In terms of the pore system, the KG Basin hydrate reservoir develops nanopores, with a relatively dispersed mineral distribution and high content of pyrite. Rich pyrite debris and foraminifera-rich paleontological shells are observed, which leads to the development of intergranular pores and provides more nanopores. The pore throat concentration and connectivity of the reservoir are high, and the permeability of sediments in the same layer varies greatly. The reason for this phenomenon is the significant difference in average pore radius and pore size contribution to pore permeability. This article provides a reference and guidance for exploring the thermodynamic stability of hydrates in sediments and the exploration and development of hydrates by characterizing the pores of hydrate reservoirs.

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Kinetics of Multicomponent Nanosize Clusters on Solid Surfaces

Cited by 2 publications

References 40 publications

Coarsening of multicomponent thin films

Coarsening of multicomponent thin films

Pore Characteristics of Hydrate-Bearing Sediments from Krishna-Godavari Basin, Offshore India

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