Micro-kinetic models provide a link between the molecular-scale mechanism of a catalytic reaction and the macro-scale observation of catalytic activity, and are central to computational catalysis. However, in real experiments it is also important to consider the reactor model to provide a direct comparison. This is particularly challenging in the case of transient kinetics experiments, such as TAP, where the steady-state assumptions that are commonly employed are no longer valid. This talk will outline recent developments toward direct simulation of TAP curves from micro-kinetic models based on the FEniCS PDE framework. The finite element approach enables direct simulation of TAP curves from based on a 1D reactor model, and the results are compared to reference implementations and experiments. Further, the FEniCS framework enables construction of adjoint models that allow automatic differentiation of the TAP response with respect to model parameters. This facilitates sensitivity analyses and efficient parameter fitting to refine micro-kinetic models through a top-down approach. The results from the most recent iteration of the TAP simulator will be presented along with a case study based on experimental results from the ammonia decomposition reaction over multiple metal alloy catalysts.

Simulation and optimization of of temporal analysis of products (TAP) curves from micro-kinetic models

2019 Spring National Meeting

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