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Title: Continuum Microkinetic Rate Theory of Lattice Systems: Formalization, Current Limitations, and a Possible Basis for Continuum Rate Theory

Abstract

A broad class of reaction networks are controlled not by any thermodynamic ensemble but by rates and are referred to as “kinetically constrained”. Here in this paper, microkinetic rate theory is extended into a model of arbitrarily complex reaction networks. This microkinetic rate theory takes a form where the constraints imposed by kinetically constrained systems apply naturally. This model is compared to numerically complete results and is shown to be quantitatively predictive. Model deviations are shown to emerge for systems with incomplete mixing. Finally, this model is analytical and may serve as a basis for device and continuum scale rate modeling.

Authors:
ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1477649
Report Number(s):
LA-UR-17-29795
Journal ID: ISSN 1089-5639
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 122; Journal Issue: 37; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS AND COMPUTING; Energy Sciences; Mathematics; Material Science

Citation Formats

Francis, Michael Frederick. Continuum Microkinetic Rate Theory of Lattice Systems: Formalization, Current Limitations, and a Possible Basis for Continuum Rate Theory. United States: N. p., 2018. Web. doi:10.1021/acs.jpca.8b06238.
Francis, Michael Frederick. Continuum Microkinetic Rate Theory of Lattice Systems: Formalization, Current Limitations, and a Possible Basis for Continuum Rate Theory. United States. doi:10.1021/acs.jpca.8b06238.
Francis, Michael Frederick. Fri . "Continuum Microkinetic Rate Theory of Lattice Systems: Formalization, Current Limitations, and a Possible Basis for Continuum Rate Theory". United States. doi:10.1021/acs.jpca.8b06238. https://www.osti.gov/servlets/purl/1477649.
@article{osti_1477649,
title = {Continuum Microkinetic Rate Theory of Lattice Systems: Formalization, Current Limitations, and a Possible Basis for Continuum Rate Theory},
author = {Francis, Michael Frederick},
abstractNote = {A broad class of reaction networks are controlled not by any thermodynamic ensemble but by rates and are referred to as “kinetically constrained”. Here in this paper, microkinetic rate theory is extended into a model of arbitrarily complex reaction networks. This microkinetic rate theory takes a form where the constraints imposed by kinetically constrained systems apply naturally. This model is compared to numerically complete results and is shown to be quantitatively predictive. Model deviations are shown to emerge for systems with incomplete mixing. Finally, this model is analytical and may serve as a basis for device and continuum scale rate modeling.},
doi = {10.1021/acs.jpca.8b06238},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 37,
volume = 122,
place = {United States},
year = {2018},
month = {9}
}

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Cited by: 1 work
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