Molecular adsorption at a well defined gas-solid interphase: Statistical Rate Theory approach

Ward, C. A.; Elmoselhi, M. B.

doi:10.1016/0039-6028(86)90049-x

Cited by 51 publications

(40 citation statements)

References 14 publications

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“…the rate of exchange at the liquid/gas interface [17][18][19], hydrogen adsorption by metals [20], electron exchange between ionic isotopes in solution [21], permeation of ionic channels in biological membranes [22], and rate of liquid evaporation [23][24][25]. Ward and co-workers were the first to show how the SRT approach can be applied to describe the kinetics of isothermal adsorption at the gas/solid interfaces [26][27][28][29], and the kinetics of thermodesorption [30]. Then a series of papers has been published during the last decade by Rudzinski and co-workers, showing how that new description can be generalized further to describe the kinetics of isothermal gas adsorption/desorption on/from energetically heterogeneous surfaces [31][32][33][34][35] as well as the kinetics of thermodesorption [36][37][38][39].…”

Section: Sorption Kinetics Governed By the Rate Of Surface Reactionsmentioning

confidence: 99%

Theoretical description of the kinetics of solute adsorption at heterogeneous solid/solution interfaces

Rudziński

Płaziński

2007

Applied Surface Science

110

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Section: Sorption Kinetics Governed By the Rate Of Surface Reactionsmentioning

confidence: 99%

Theoretical description of the kinetics of solute adsorption at heterogeneous solid/solution interfaces

Rudziński

Płaziński

2007

Applied Surface Science

110

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“…If the solid is large enough that the adsorption takes place isothermally, SRT may be used to formulate the expression for the instantaneous rate of adsorption, J. In this case, one finds 7,12,14,15 …”

Section: Adsorption Rate In An Isolated Systemmentioning

confidence: 99%

“…The exception is the ''adsorption cross section'' that has been previously defined. 12,14,15 In an isolated system, SRT leads to the prea͒ Present address: Department of Chemistry and Materials Engineering, Univ. Alberta, Edmonton, Canada T6G 26G.…”

Section: Introductionmentioning

confidence: 99%

“…The SRT approach shows promise of being successful, but it has not been fully tested previously. Since it was first proposed in an elementary form in 1977, 5 it has been placed on firmer theoretical grounds 6,7 and applied to examine the rates of gas absorption at a liquid-gas interface, [8][9][10] hydrogen absorption by metals, 11 electron exchange between ionic isotopes in solution, 6,12 permeation of ionic channels in biological membranes, 13 and both nondissociative 12,14,15 and dissociative 14,16 adsorption kinetics in isothermal, isobaric systems. In each case, the SRT approach led to improvements in the theoretical description of the rate process.…”

Section: Introductionmentioning

confidence: 99%

“…2,4 Statistical rate theory is being developed with the objective of filling this need. [5][6][7][8][9][10][11][12][13][14][15][16] In this approach, a thermodynamically isolated system is considered and the transition probability concept is used to construct the expression for the rate of molecular transport. If this approach is successful, the material properties of a particular pair of macroscopic phases could be tabulated and used in the governing equations for predicting the rate of molecular transport across the interface in any circumstance.…”

Section: Introductionmentioning

confidence: 99%

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Statistical rate theory description of beam-dosing adsorption kinetics

Elliott

Ward

1997

The Journal of Chemical Physics

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Absolute rate theory and the sticking probability approach have been previously examined as possible means of predicting the rate of adsorption. However, when applied to examine adsorption kinetics, they have been found not to contain the coverage and pressure dependence required for several important systems including CO–Ni(111). Statistical rate theory (SRT) is being developed with the objective of predicting the rate of molecular (or atomic) transport across the interface between macroscopic phases in terms of experimentally controllable variables and material properties of the two phases. Previous applications of SRT to adsorption have been limited to systems for which both the gas phase pressure and the temperature could be assumed to be constant. Herein, the SRT approach is extended to systems in which the number of molecules in the system (and hence the gas phase pressure) is not constant. To examine this extension, SRT is used to formulate the equations governing the rate of adsorption in isothermal, beam-dosing experiments. These equations are then combined with the values of certain material properties that have previously been established and a hypothesis that the value of the equilibrium adsorption cross section is given by the area of an adsorption site. The kinetic data for CO adsorbing on Ni(111) data reported by three different laboratories are then examined. For each set of experimental data, constants had to be inferred that were related to the experimental apparatus used and as such they were not expected to have any coverage or pressure dependence. The good agreement found between the predicted and measured adsorption kinetics indicates that all of the necessary coverage and pressure dependence was explicitly predicted from the SRT approach.

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