Sabatier Principle-Driven Single-Atom Coordination Engineering for Enhanced Fenton-Like Catalysis

Area of Science:

• Materials Science
• Environmental Chemistry
• Catalysis

Background:

• Single-atom catalysts (SACs) are crucial for Fenton-like reactions but lack design guidelines.
• The Sabatier principle offers a theoretical framework for optimizing catalyst performance.

Purpose of the Study:

• To explore the Sabatier relationship in Fenton-like catalysis by engineering SACs with varied d-band centers.
• To establish guidelines for designing high-performance SACs for pollutant degradation.

Main Methods:

• Single-atom coordination engineering to create SACs with diverse d-band centers.
• Investigating the correlation between d-band centers and catalytic activity.
• Utilizing theoretical and experimental approaches to analyze reaction mechanisms.

Main Results:

• A volcanic correlation was identified between d-band centers and catalytic activity.
• Moderate d-band centers and peroxymonosulfate adsorption energy minimize reaction barriers for singlet oxygen generation.
• The Fe-N2O2/C catalyst achieved a degradation rate constant of 1.89 min⁻¹, significantly outperforming other SACs.

Conclusions:

• The Sabatier principle effectively guides the design of SACs for enhanced Fenton-like catalysis.
• Optimized SACs demonstrate superior pollutant degradation efficiency and environmental stability.
• This work provides a pathway for developing advanced catalysts for eco-friendly environmental remediation.