Finely Tailoring Metal-Support Interactions via Transient High-Temperature Pulses

Area of Science:

• Materials Science
• Catalysis
• Surface Chemistry

Background:

• Metal-support interactions (MSI) are vital for catalyst performance but difficult to control at the atomic scale.
• Suboptimal MSI (too weak or too strong) leads to reduced catalytic activity and stability.
• Developing methods for precise MSI control is crucial for advanced catalyst design.

Purpose of the Study:

• To develop a method for finely tuning metal-support interactions (MSI) at the atomic scale.
• To investigate the formation of different MSI types and their impact on catalytic properties.
• To optimize MSI for enhanced catalytic activity and stability in heterostructured catalysts.

Main Methods:

• Utilized temporal-precise transient high-temperature pulse heating to modify Pt/CeO2 catalysts.
• Systematically varied pulse duration and atmosphere to control metal-support interface reconstruction.
• Employed theoretical calculations to understand electronic structure modifications and reaction mechanisms.

Main Results:

• Successfully created two distinct MSI types: strong MSI (SMSI, Pt@CeO2) and reactive MSI (RMSI, Pt5Ce@CeO2).
• Pt5Ce@CeO2 with RMSI demonstrated exceptional performance in alkaline hydrogen evolution (overpotential of -29 mV, stable for >300 h).
• Alloying Pt with Ce (Pt5Ce) modified Pt's electronic structure, optimizing intermediate adsorption/dissociation and reducing reaction barriers.

Conclusions:

• Temporal-precise transient heating offers a controllable strategy for tuning MSI.
• The Pt5Ce@CeO2 system with RMSI shows significant potential for efficient and durable hydrogen evolution catalysis.
• This approach provides valuable insights for designing heterostructured catalysts with tailored MSI for diverse applications.