Renewable power sources (e.g., wind) are now cost-competitive with fossil-fuel derived power, but these sources of renewable energy are located far from urban centers, necessitating methods to store and transport energy. Distributed production of chemical energy liquids such as ammonia is one potential solution for providing storable, fungible, and commodity energy liquids. Downsizing current industrial processes to small modular units is currently inhibited by poor catalytic performance. For example, intense reactor operating conditions (400°C, &gt; 150 atm) are required to achieve adequate reaction rates for thermocatalytic ammonia synthesis. As an alternative, we propose a new catalyst design strategy, programmable catalysis, to shift reactions away from equilibrium and increase reaction rates. In this strategy, reaction directionality is controlled through use of perturbed catalyst surfaces (e.g., electronic and steric manipulation); by changing the electronic occupation of the catalyst, catalyst-adsorbate interactions are temporally tuned. Through microkinetic modeling of a reversible catalytic reaction, we define the catalytic parameter space for tuning these programmable catalysts to optimize product selectivity. We identify the design parameters (e.g., amplitude, frequency, linear scaling parameters) for these systems and describe a robust descriptor that can predict the overall reaction directionality without the need for full simulations.

Programmable catalysts: A kinetic strategy for controlling reaction product distribution

ACS Spring 2022

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