Micki: A python-based object-oriented microkinetic modeling code.

Abstract

We have developed a flexible, general-purpose microkinetic modeling code, Micki, to analyze complex, heterogeneously catalyzed chemical reactions based upon first-principles calculations. This Python-based code is modular and object oriented, framing the development of microkinetic models in familiar chemical terms. We also present novel approaches, incorporated into Micki, to describe diffusion limited reactions, multidentate bindings, thermodynamically consistent lateral interactions, and Brønsted-Evans-Polanyi estimates of changes in barrier heights. Micki has built-in modules for subsequent analysis of microkinetic models, including degree of rate control and rate order. As a demonstration of the power and flexibility of the code, we build a microkinetic model for the water-gas shift reaction and compare to previously published experimental results and microkinetic models, showing that Micki can quantitatively reproduce experimental turnover frequencies with minimal empirical optimization.