Dataset for Modified Energy Span Analysis Reveals Heterogeneous Catalytic Kinetics

Published: 8 April 2022| Version 1 | DOI: 10.17632/htfngy4kch.1
Maximilian Cohen,


Publication available online at: Mechanistic modeling is a cornerstone of catalyst development generally conducted with microkinetic models or density functional theory-based energy profiles. We extend the energy span model of homogeneous catalysis to heterogeneous systems by introducing the modified energy span analysis (MESA) model by implementing collision theory and gas-phase concentration effects. We determine analytically turnover frequencies, coverages, rate-determining steps, apparent activation energies, and reaction orders in agreement with microkinetic and kinetic Monte Carlo simulations. The model applies to discrete catalyst state systems, including single-atom catalysts, homogeneous systems, and microporous materials. A generalizable rate expression is derived for reactor modeling or mechanistic insights from solely experimentally measured reaction orders. We illustrate MESA on three published mechanisms and reveal unexpected phenomena absent in traditional energy span profiles.



University of Delaware


Chemical Reaction Kinetics, Heterogeneous Catalysis, Catalytic Mechanism, Parameter Estimation