The Catalytic Mechanics of Dynamic Surfaces: Stimulating Methods for Promoting Catalytic Resonance
Manish Shetty, Amber Walton, Sallye R. Gathmann, M. Alexander Ardagh, Joshua Gopeesingh, Joaquin Resasco, Turan Birol, Qi Zhang, Michael Tsapatsis, Dionisios G. Vlachos, Phillip Christopher, C. Daniel Frisbie, Omar Abdelrahman, Paul J. Dauenhauer
Abstract
Transformational catalytic performance\nin rate and selectivity\nis obtainable through catalysts that change on the time scale of catalytic\nturnover frequency. In this work, dynamic catalysts are defined in\nthe context and history of forced and passive dynamic chemical systems,\nwith the classification of unique catalyst behaviors based on temporally\nrelevant linear scaling parameters. The conditions leading to the\ncatalytic rate and selectivity enhancement are described as modifying\nthe local electronic or steric environment of the active site to independently\naccelerate sequential elementary steps of an overall catalytic cycle.\nThese concepts are related to physical systems and devices that stimulate\na catalyst using light, vibrations, strain, and electronic manipulations\nincluding electrocatalysis, back-gating of catalyst surfaces, and\nintroduction of surface electric fields via solid electrolytes and\nferroelectrics. These catalytic stimuli are then compared for the\ncapability to improve catalysis across some of the most important\nchemical challenges for energy, materials, and sustainability.