(205f) Dynamic Modulation of Catalyst Electronic Structure to Enhance Reaction Rates
In this talk, we present an alternative approach where catalyst electronic structure, and therefore binding properties, are varied as a function of time . The effectiveness of this approach was demonstrated using a CSTR with a model A â B system that has three elementary steps: (i) adsorption of A, (ii) surface reaction of A* â B*, and (iii) desorption of B. Binding properties were varied with a square, sinusoidal, triangle, or saw-tooth waveform with a specified oscillation frequency (fosc , [=]Hz) and amplitude (ÎU, [=] eV). Experimentally, this electronic structure oscillation can be implemented with back-gate voltage, applied strain, and varying feed pressure/composition. Computationally, we found that steady state rates depend strongly on the frequency and amplitude. For moderate oscillation amplitudes (0.5-1.5 eV), the steady state rate has a resonance frequency range between 103 -107 Hz where the rate plateaus at up to 10,000x greater than the Sabatier maximum. With practical implementation in mind, various oscillation waveform were compared to assess their effectiveness. Square waveform had the highest performance but the sinusoidal waveform also led to high rate enhancement.
 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