A Breakthrough in Formic Acid Oxidation by a Dual-Atomic Ir-N₄/Pt-N₄ Catalyst via Parallel Reaction Pathways Under...

Area of Science:

• Heterogeneous catalysis
• Materials science
• Electrochemistry

Background:

• Single-atom catalysts (SACs) face challenges in multi-atomic molecule oxidation due to simple active sites and slow reaction pathways.
• Existing catalysts exhibit sluggish desorption-charge transfer, limiting efficiency in complex oxidation reactions.

Purpose of the Study:

• To develop an efficient dual-atom catalyst (Ir1-Pt1 NC) with Ir-N4/Pt-N4 active sites for enhanced formic acid oxidation (FAOR).
• To investigate a dual-pathway mechanism and the effect of an over-boiling point environment on catalytic performance.

Main Methods:

• Synthesis of atomically dispersed Ir-N4/Pt-N4 dual-isolated coordination structure.
• Electrocatalytic testing under over-boiling point conditions.
• Molecular dynamics (MD) simulations to analyze hydrogen bonding and molecular diffusion.

Main Results:

• The Ir1-Pt1 NC catalyst demonstrated a mass activity of 125.9 A mg-1, significantly outperforming state-of-the-art SACs and commercial Ir/C.
• A parallel dual-pathway mechanism was established, with Pt activating H adsorption and Ir binding carbonyl groups.
• Over-boiling point operation effectively weakened hydrogen bonds in formic acid solutions, enhancing molecular diffusion and catalytic kinetics.

Conclusions:

• The "dual-atomic catalyst with over-boiling point hydrogen bond dissociation" strategy offers a new paradigm for catalyst design and environmental regulation.
• This approach achieves unprecedented catalytic performance for FAOR and holds promise for degrading other small organic molecules.
• The study highlights a universal "structure + environment" dual-regulation strategy for advanced catalysis.