Campus Units
Chemistry, Physics and Astronomy, Ames Laboratory
Document Type
Article
Publication Version
Published Version
Publication Date
2010
Journal or Book Title
Journal of Chemical Physics
Volume
132
Issue
15
First Page
154102-1
Last Page
154102-11
DOI
10.1063/1.3361663
Abstract
We analyze a model for polymerization at catalytic sites distributed within parallel linear pores of a mesoporous material. Polymerization occurs primarily by reaction of monomers diffusing into the pores with the ends of polymers near the pore openings. Monomers and polymers undergo single-file diffusion within the pores. Model behavior, including the polymer length distribution, is determined by kinetic Monte Carlo simulation of a suitable atomistic-level lattice model. While the polymers remain within the pore, their length distribution during growth can be described qualitatively by a Markovian rate equation treatment. However, once they become partially extruded, the distribution is shown to exhibit non-Markovian scaling behavior. This feature is attributed to the long-tail in the “return-time distribution” for the protruding end of the partially extruded polymer to return to the pore, such return being necessary for further reaction and growth. The detailed form of the scaled length distribution is elucidated by application of continuous-time random walk theory.
Rights
Copyright 2010 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.
Copyright Owner
American Institute of Physics
Copyright Date
2010
Language
en
File Format
application/pdf
Recommended Citation
Liu, Da-Jiang; Chen, Hung-Ting; Lin, Victor S.-Y.; and Evans, James W., "Polymer length distributions for catalytic polymerization within mesoporous materials: Non-Markovian behavior associated with partial extrusion" (2010). Physics and Astronomy Publications. 193.
https://lib.dr.iastate.edu/physastro_pubs/193
Comments
The following article appeared in Journal of Chemical Physics 132, 15 (2010): 154102 and may be found at doi: 10.1063/1.3361663.