ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 653 - 663

Published: Dec. 23, 2024

Programmable catalysts exhibiting forced oscillation in the free energy of reacting surface species were simulated to understand general mechanisms leading efficient use input energy. Catalytic ratchets with either positive or negative adsorbate scaling exhibited conditions both high and low turnover efficiency, yielding catalytic frequencies close significantly lower than applied catalyst frequency, respectively. The "effective rate", defined as product frequency efficiency (ηTOE), was limited via two mechanisms: a leaky ratchet existed when molecules repeatedly traversed backward through transition state upon oscillation, while participation reduced formation gas-phase final due coverage. A single maximum effective rate "resonance frequency" provided combined benefit for efficiency.

Language: Английский