Over the past 60 years, intensive catalyst design and reaction engineering have brought catalysis research to the brink of optimized industrial production rates. Most relevant reaction chemistries have been thoroughly optimized to the point where incremental catalysis research is no longer funded. However, even fully optimized catalysts are quite ineffective for vital, difficult reactions such as NH3 synthesis or CH4 oxidation to methanol. The rate of production for a given reaction is limited by the Sabatier principle, which states that optimum reactivity is achieved at intermediate binding of reactants and products onto the catalyst. Our approach of dynamic heterogeneous catalysis leverages ‘Catalytic Resonance Theory’ to achieve high rate enhancement several orders of magnitude above the Sabatier speed limit. This may be achieved by varying the binding properties of the catalyst with time. Catalytic Resonance Theory proposes that the optimum frequency to vary binding energies is similar to the speed of the elementary steps occurring on the catalyst surface. The effects of dynamic catalysts on reaction performance are studied using a combination of numerical simulation, computational chemistry (DFT), and experiment. Numerical simulations in Matlab 2019a and 2019b of example reaction networks with a single reaction (A-to-B) and parallel reactions (A-to-B & A-to-C) demonstrate that Catalytic Resonance Theory conceptually leads to high rate, conversion, and selectivity enhancement. Performance is controlled by new dynamic tuning handles including the oscillation frequency ([=] Hz), amplitude ([=] eV), and amplitude endpoints ([=] eV). Reaction rate enhancement of 1,000-10,000x were achieved on single and parallel reaction networks at moderate amplitudes ~0.5-1.0 eV. The degree of rate enhancement above the Sabatier speed limit depends on the Brønsted-Evans-Polanyi (BEP) and linear scaling relationships for the reaction chemistry. Higher BEP proportionality constants (α) close to 1.0 lead to higher rate enhancement and high linear scaling proportionally constants (γ) &gt;1.0 allow us to rapidly produce the desired product. Both of these findings imply that probe reactions such as molecular decomposition and dehydrogenation have high potential enhancement. Future work includes using DFT calculations and experiment to explore the sensitivity of common adsorbates (CO, NO, N, O, OH) to external stimuli such as stress/strain, electric fields, and lasers/plasmonics.

Catalytic resonance theory: Breaking the Sabatier speed limit via surface frequency response

Macromolecular Chemistry: The Second Century

[Author Benefits](https://scimeetings.acs.org/?utm_source=pubs_content_marketing&utm_medium=website&utm_campaign=0320_MCF_NPI_Launch_Spring_Homepage&ref=pubs_content_marketing)

[How to use SciMeetings](https://storage.googleapis.com/dl.morressier.com/acs/SciMeetings-ACSSpring2020-HowToGuide_M3020-Final.pdf)

[Frequently Asked Questions](https://storage.googleapis.com/dl.morressier.com/acs/SciMtng_ACSNMSp2020_FAQ_M3120_Final.pdf)

ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.