Catalytic conversion reactions in nanoporous systems with concentration-dependent selectivity: Statistical mechanical modeling.
Statistical mechanical modeling is developed to describe a catalytic conversion reaction A→B^{c} or B^{t} with concentration-dependent selectivity of the products, B^{c} or B^{t}, where reaction occurs inside catalytic particles traversed by narrow linear nanopores. The associated restricted diffusive transport, which in the extreme case is described by single-file diffusion, naturally induces strong concentration gradients. Furthermore, by comparing kinetic Monte Carlo simulation results with analytic treatments, selectivity is shown to be impacted by strong spatial correlations induced by restricted diffusivity in the presence of reaction and also by a subtle clustering of reactants, A.
Ames Laboratory-USDOE, Iowa State University, Ames, Iowa 50011, USA.|Department of Physics & Astronomy, Iowa State University, Ames, Iowa 50011, USA.
Andrés
A
García
Ames Laboratory-USDOE, Iowa State University, Ames, Iowa 50011, USA.|Department of Mathematics, Iowa State University, Ames, Iowa 50011, USA.
Jing
J
Wang
Ames Laboratory-USDOE, Iowa State University, Ames, Iowa 50011, USA.|Department of Chemistry, Iowa State University, Ames, Iowa 50011, USA.
Theresa L
TL
Windus
Ames Laboratory-USDOE, Iowa State University, Ames, Iowa 50011, USA.|Department of Chemistry, Iowa State University, Ames, Iowa 50011, USA.
Aaron D
AD
Sadow
Ames Laboratory-USDOE, Iowa State University, Ames, Iowa 50011, USA.|Department of Physics & Astronomy, Iowa State University, Ames, Iowa 50011, USA.|Department of Mathematics, Iowa State University, Ames, Iowa 50011, USA.
James W
JW
Evans