Sabatier Principle Driving Interface Defect Engineering on 3D Graphene-Like Encapsulated Cobalt Structure for Hydrogenation Reaction.

Establishing structural defects is a perspective way to increase the catalytic hydrogenation reaction. Toward Sabatier optimization for hydrogenation reaction with defect density offers guidance for designing optimal catalysts with the highest performance. A controllable synthesis strategy is reported for Co@NC-x catalyst induced by defect density. A series of N-doped carbon-based defective Co@NC-x catalysts with different defect densities ranging from 1.5 × 10 to 1.9 × 10 cm via high-temperature sublimation strategy is obtained. The results show that the volcano curves are observed between defect density and catalytic hydrogenation performance with a summit at a moderate defect density of 1.7 × 10 cm, matched well with Sabatier phenomenon. Remarkably, the defect density on the graphene-like shell serves as descriptor to the adsorbate state and consequently the catalytic activity. However, to the best of knowledge, the Sabatier phenomenon in hydrogenation reactions at the defect scale in 3D graphene-like encapsulated metal (3D-GEM) catalysts has not been reported. This work highlights the meaning of defect-density effect on catalytic hydrogenation reaction, supplying meaningful guidance for the rational design of more efficient and durable defective 3D-GEM catalyst.