Confined Mn Single-Atom Anchoring on Fullerene Monolayers With Enhanced Electron-Buffering for Selective CO Electroreduction

The present work investigated the binding of atomically dispersed transition metals to the 2D fullerene quasihexagonal phase C₆₀ (qhp-C₆₀) framework and the catalytic performance of the corresponding single/dual-sided single-atom catalysts for CO electroreduction by means of density functional theory calculations. Compared to isolated C₆₀ molecules, the qhp-C₆₀ framework not only effectively inhibits metal aggregation through its unique confining nanocages and stronger metal–substrate interactions, but also enhances the catalytic activity and selectivity by a more efficient electron-buffering effect. Among all the metal centers examined, Mn was identified as the most promising candidate for selective CO-to-methane conversion.