Campus Units

Chemistry, Mathematics, Physics and Astronomy, Ames Laboratory

Document Type

Article

Publication Version

Published Version

Publication Date

7-2014

Journal or Book Title

Physical Review Letters

Volume

113

Issue

3

First Page

1

Last Page

5

DOI

10.1103/PhysRevLett.113.038301

Abstract

Inhibited passing of reactant and product molecules within the linear pores of nanoporous catalytic materials strongly reduces reactivity. The dependence of the passing propensity P on pore radius R is analyzed utilizing Langevin dynamics to account for solvent effects. We find that P∼(R−Rc)σ, where passing is sterically blocked for R≤Rc, with σ below the transition state theory value. Deeper insight comes from analysis of the corresponding high-dimensional Fokker-Planck equation, which facilitates an effective small-P approximation, and dimensional reduction enabling utilization of conformal mapping ideas. We analyze passing for spherical molecules and also assess the effect of rotational degrees of freedom for elongated molecules.

Comments

This article is from Physical Review Letters 113 (2014): 038301, doi:10.1103/PhysRevLett.113.038301. Posted with permission.

Copyright Owner

American Physical Society

Language

en

File Format

application/pdf

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