Catalytic conversion reactions in nanoporous systems with concentration-dependent selectivity: Statistical mechanical modeling

Garcia, Andres; Wang, Jing; Windus, Theresa L.; Sadow, Aaron D.; Evans, James W.

doi:10.1103/physreve.93.052137

Cited by 2 publications

(6 citation statements)

References 31 publications

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“…The corresponding estimate of tracer diffusivity is D tr (pair) = (2 − X 0 )(2 + X 0 ) −1 D tr (site) [19]. Thus, for large L, we find that D tr (max)/D tr (pair) = 0.907 (0.650) for X 0 = 0.2 (0.8), (25) so indeed this pair approximation captures the maximum effective tracer diffusivity significantly better than the site approximation.…”

Section: Generalized Tracer Diffusivity For Sfdmentioning

confidence: 68%

“…The generalized tracer diffusivity provides a comprehensive characterization of transport within the pore, and has been shown to be invaluable in elucidating behavior of more complex reaction-diffusion processes [19,20,25,30]. From the broader perspective on nonequilibrium systems and steady states, it is instructive to provide a complete characterization of these states.…”

Section: Discussionmentioning

confidence: 99%

“…Perhaps closer to the TCP scenario are finite or semi-infinite lattice-gas reaction-diffusion systems with SFD or less restrictive inhibited passing. In these systems, reaction induces subtle positive clustering correlations [19,25].…”

Section: Introductionmentioning

confidence: 99%

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Tracer counterpermeation analysis of diffusivity in finite-length nanopores with and without single-file dynamics

Ackerman

Evans

2017

Phys. Rev. E

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We perform a tracer counterpermeation (TCP) analysis for a stochastic model of diffusive transport through a narrow linear pore where passing of species within the pore is inhibited or even excluded (single-file diffusion). TCP involves differently labeled but otherwise identical particles from two decoupled infinite reservoirs adsorbing into opposite ends of the pore, and desorbing from either end. In addition to transient behavior, we assess steady-state concentration profiles, spatial correlations, particle number fluctuations, and diffusion fluxes through the pore. From the profiles and fluxes, we determine a generalized tracer diffusion coefficient Dtr(x), at various positions x within the pore. Dtr(x) has a plateau value in the pore center scaling inversely with the pore length, but it is enhanced near the pore openings. The latter feature reflects the effect of fluctuations in adsorption and desorption, and it is also associated with a nontrivial scaling of the concentration profiles near the pore openings. Disciplines Biological and Chemical Physics | Engineering Physics | Nanoscience and Nanotechnology CommentsThis article is from Physical Review E 95 (2017) We perform a tracer counterpermeation (TCP) analysis for a stochastic model of diffusive transport through a narrow linear pore where passing of species within the pore is inhibited or even excluded (single-file diffusion). TCP involves differently labeled but otherwise identical particles from two decoupled infinite reservoirs adsorbing into opposite ends of the pore, and desorbing from either end. In addition to transient behavior, we assess steady-state concentration profiles, spatial correlations, particle number fluctuations, and diffusion fluxes through the pore. From the profiles and fluxes, we determine a generalized tracer diffusion coefficient D tr (x), at various positions x within the pore. D tr (x) has a plateau value in the pore center scaling inversely with the pore length, but it is enhanced near the pore openings. The latter feature reflects the effect of fluctuations in adsorption and desorption, and it is also associated with a nontrivial scaling of the concentration profiles near the pore openings.

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Section: Generalized Tracer Diffusivity For Sfdmentioning

confidence: 68%

Section: Discussionmentioning

confidence: 99%

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Tracer counterpermeation analysis of diffusivity in finite-length nanopores with and without single-file dynamics

Ackerman

Evans

2017

Phys. Rev. E

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“…These serve as "boundary conditions." The fluxes (2), which reflect the feature that hopping occurs only to neighboring empty cells, cannot be written in terms of single-cell concentrations due to spatial correlations between occupancy of different cells [11,[20][21][22][23]36]. Thus (1) is not closed, but rather is just the lowestorder equation in a hierarchy [11].…”

Section: B Heterogeneous Master Equationsmentioning

confidence: 99%

“…The triplet approximation writes quartets in terms of triplets, etc. However, even these higher-order truncation approximations fail to accurately capture behavior given the strong correlations induced by the SFD constraint [11,36]. See the Appendix for a more detailed discussion, and also the Supplemental Material [37] for additional results.…”

Section: B Heterogeneous Master Equationsmentioning

confidence: 99%

Generalized hydrodynamic analysis of transport through a finite open nanopore for two-component single-file systems

et al. 2020

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Single-file diffusion (SFD) in finite open nanopores is characterized by nonzero spatially varying tracer diffusion coefficients within a generalized hydrodynamic description. This contrasts with infinite SFD systems where tracer diffusivity vanishes. In standard tracer counterpermeation (TCP) analysis, two reservoirs, each containing a different species, are connected to opposite ends of a finite pore. We implement an extended TCP analysis to allow the two reservoirs to contain slightly different mixtures of the two species. Then, determination of diffusion fluxes through the pore allows extraction of diffusion coefficients for near-constant partial concentrations of the two species. This analysis is applied for a lattice-gas model describing twocomponent SFD through a finite linear pore represented by a one-dimensional array of cells. Two types of particles, A and B, can hop only to adjacent empty cells with generally different rates, h A and h B . Particles are noninteracting other than exclusion of multiple cell occupancy. Results reveal generalized hydrodynamic tracer diffusion coefficients which adopt small values inversely proportional to pore length in the pore center, but which are strongly enhanced near pore openings.

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Catalytic conversion reactions in nanoporous systems with concentration-dependent selectivity: Statistical mechanical modeling

Cited by 2 publications

References 31 publications

Tracer counterpermeation analysis of diffusivity in finite-length nanopores with and without single-file dynamics

Tracer counterpermeation analysis of diffusivity in finite-length nanopores with and without single-file dynamics

Generalized hydrodynamic analysis of transport through a finite open nanopore for two-component single-file systems

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