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

Area of Science:

• Materials Science
• Catalysis
• Chemical Engineering

Background:

• Structural defects in catalysts can significantly influence reaction rates.
• Optimizing defect density is crucial for maximizing catalytic hydrogenation performance.
• The Sabatier principle guides catalyst optimization by considering reaction intermediates.

Purpose of the Study:

• To develop a controllable synthesis strategy for N-doped carbon-based defective Co@NC-x catalysts.
• To investigate the relationship between defect density and catalytic hydrogenation performance.
• To explore the role of defect density as a descriptor in 3D graphene-like encapsulated metal (3D-GEM) catalysts.

Main Methods:

• High-temperature sublimation strategy to synthesize Co@NC-x catalysts with varying defect densities (1.5 × 10^11 to 1.9 × 10^11 cm^-2).
• Evaluation of catalytic hydrogenation performance across the synthesized catalysts.
• Analysis of the correlation between defect density and catalytic activity.

Main Results:

• A volcano curve relationship was observed between defect density and catalytic hydrogenation performance.
• Optimal catalytic performance was achieved at a moderate defect density of 1.7 × 10^11 cm^-2, consistent with the Sabatier phenomenon.
• Defect density on the graphene-like shell acts as a descriptor for adsorbate states and catalytic activity.

Conclusions:

• Defect density is a critical factor for optimizing catalytic hydrogenation in Co@NC-x catalysts.
• The Sabatier phenomenon is demonstrated at the defect scale in 3D-GEM catalysts.
• This research provides guidance for designing efficient and durable defective 3D-GEM catalysts.