Understanding the Activity of Carbon-Based Single-Atom Electrocatalysts from Ab Initio Simulations

Heterogeneous single-atom catalysis has attracted great research interest in recent years. The atomically dispersed metal atoms, which are generally active sites in single-atom catalysts, could result in unconventional reaction mechanisms due to the site confinement of reaction intermediates. Their coordination environments substantially affect their activities through tuning the adsorption of reaction intermediates. Two kinds of coordination effects were discussed here: intrinsic coordination and dynamic coordination. The intrinsic coordination is formed in the synthesis process of the catalyst, and the dynamic coordination refers to the in situ coordination of an atom or a group introduced during catalysis. The charge capacity of the active site and solvation effect also play an important role in the adsorption of reactants and intermediates on single-atom catalysts.

Automated summary

Research interest has been increasing in heterogeneous single-atom catalysis, where the atomically dispersed metal atoms act as active sites that can lead to unconventional reaction mechanisms due to site confinement. Coordination environments significantly influence the activity of single-atom catalysts by tuning the adsorption of reaction intermediates.