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Molecular iridium catalysts immobilized in metal-organic frameworks (MOFs) were positioned in the condensing chamber of a Soxhlet extractor for efficient CO hydrogenation. Droplets of hot water seeped through the MOF catalyst to create dynamic gas/liquid interfaces which maximize the contact of CO, H, HO, and the catalyst to achieve a high turnover frequency of 410 h under atmospheric pressure and at 85 °C. H/D kinetic isotope effect measurements and density functional theory calculations revealed concerted proton-hydride transfer in the rate-determining step of CO hydrogenation, which was difficult to unravel in homogeneous reactions due to base-catalyzed H/D exchange.

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Electrode potential is the key factor for controlling electrocatalytic reactions at electrochemical interfaces, and moreover, it is also known that the pH and solutes (e.g., cations) of the solution have prominent effects on electrocatalysis. Understanding these effects requires microscopic information on the electrochemical interfaces, in which theoretical simulations can play an important role. This Perspective summarizes the recent progress in method development for modeling electrochemical interfaces, including different methods for describing the electrolytes at the interfaces and different schemes for charging up the electrode surfaces. In the final section, we provide an outlook for future development in modeling methods and their applications to electrocatalysis.