Number of sites-based solver for determining coverages from steady-state mean-field micro-kinetic models. 2024

Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
CatTheory, Department of Physics, Technical University of Denmark, Kgs. Lyngby, Denmark.

Kinetic models parameterized by ab-initio calculations have led to significant improvements in understanding chemical reactions in heterogeneous catalysis. These studies have been facilitated by implementations which determine steady-state coverages and rates of mean-field micro-kinetic models. As implemented in the open-source kinetic modeling program, CatMAP, the conventional solution strategy is to use a root-finding algorithm to determine the coverage of all intermediates through the steady-state expressions, constraining all coverages to be non-negative and to properly sum to unity. Though intuitive, this root-finding strategy causes issues with convergence to solution due to these imposed constraints. In this work, we avoid explicitly imposing these constraints, solving the mean-field steady-state micro-kinetic model in the space of number of sites instead of solving it in the space of coverages. We transform the constrained root-finding problem to an unconstrained least-squares minimization problem, leading to significantly improved convergence in solving micro-kinetic models and thus enabling the efficient study of more complex catalytic reactions.

UI MeSH Term Description Entries

Related Publications

Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
October 1972, FEBS letters,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
November 2011, Physical review. E, Statistical, nonlinear, and soft matter physics,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
July 2017, The Journal of chemical physics,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
January 1992, Physical review. A, Atomic, molecular, and optical physics,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
August 2018, Physical chemistry chemical physics : PCCP,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
July 2002, Physical review. E, Statistical, nonlinear, and soft matter physics,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
January 2015, IEEE transactions on cybernetics,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
November 1975, Journal of theoretical biology,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
September 2011, Journal of fluorescence,
Sudarshan Vijay, and Hendrik H Heenen, and Aayush R Singh, and Karen Chan, and Johannes Voss
October 2011, Journal of physics. Condensed matter : an Institute of Physics journal,
Copied contents to your clipboard!