(560jf) Dynamic Catalysis and Surface Resonance for Turnover Frequency Enhancement
Using a CSTR model in Matlab, a model system with A â B and three elementary steps: (i) adsorption of A, (ii) surface reaction of A* â B*, and (iii) desorption of B was studied. The catalyst binding properties were varied using a square, sinusoidal, triangle, or saw-tooth waveform with a specified oscillation frequency (fosc , [=] Hz) and amplitude (ÎU, [=] eV). The dynamic steady state rate was found to be a strong function of frequency and amplitude. For moderate amplitudes between 0.5-1.5 eV, there is a resonance frequency range between 103 -107 Hz where steady state rates level off at 100-10,000x the Sabatier maximum. With practicality in mind, the oscillation waveform was tested at the same frequency and amplitude to assess their effectiveness in rate enhancement. Square waveform were the highest performing but sinusoidal waveform still led to high rate enhancement. These new process handles of frequency, amplitude, and waveform allow for reaction engineering to greatly improve process performance.
 M. A. Ardagh, O. A. Abdelrahman, P. J. Dauenhauer, âPrinciples of Dynamic Heterogeneous Catalysis: Surface Resonance and Turnover Frequency Responseâ ChemRxiv Preprint, 2019. doi.org/10.26434/chemrxiv.7790009.v1