Collaboration between a Pt-dimer and neighboring Co-Pd atoms triggers efficient pathways for oxygen reduction...

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• Developing cost-effective electrocatalysts for the oxygen reduction reaction (ORR) is crucial for fuel cell technology adoption.
• Existing catalysts often face trade-offs between performance and economic viability.
• Mimicking advanced nanocatalyst structures computationally is key to catalyst design.

Purpose of the Study:

• To design and investigate a novel diatomic platinum-cluster (Pt-dimer) electrocatalyst on a cobalt-palladium (Co/Pd) bimetallic surface.
• To understand the local-regional collaboration pathways governing the oxygen reduction reaction (ORR) on this new catalyst model.
• To assess the potential for developing economical and high-performance catalysts using computational methods.

Main Methods:

• Utilizing density functional theory (DFT) to model a unique diatomic Pt-cluster on a Co/Pd bimetallic slab (Co@Pd-Pt2).
• Systematically investigating local-regional collaboration pathways for the ORR.
• Calculating adsorption energy variations, reaction coordinates, and intraparticle charge injection.

Main Results:

• The Pt-dimer induces local differentiation on the Co@Pd surface through ligand and geometric effects.
• Adsorption energy gradients were formed, facilitating the relocation of ORR adsorbates.
• The Co@Pd-Pt2 system demonstrated superior ORR performance due to novel local synergetic collaboration around the Pt-dimer.

Conclusions:

• The proposed Co@Pd-Pt2 model with a diatomic Pt-cluster exhibits excellent ORR performance.
• Local synergetic collaboration around the Pt-dimer is key to enhanced catalytic activity.
• DFT assessments can guide the development of economical, high-performance catalysts for various reactions.