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

Single-atom catalysts (SACs) are widely employed in Fenton-like catalysis, yet guidelines for their high-performance design remain elusive. The Sabatier principle provides guidance for the ideal catalyst with the highest activity. Herein, the study meticulously engineered a series of SACs featuring a broad distribution of d-band center through single-atom coordination engineering, facilitating a comprehensive exploration of the Sabatier relationship in Fenton-like catalysis. A volcanic correlation between d-band centers and catalytic activity is identified. Theoretical and experimental results show that moderate d-band center and peroxymonosulfate adsorption energy can lead to the lowest reaction barriers in the rate-determining step for generating singlet oxygen, thus enhancing catalytic efficiency toward the Sabatier optimum. As proof of concept, the Fe-N₂O₂/C catalyst demonstrates a degradation rate constant of 1.89 min^-1, surpassing Fe-N₄/C by 3.2 times and Fe-O₄/C by 272 times. Moreover, Fe-N₂O₂/C shows exceptional tolerance to various environmental challenges, providing opportunities for achieving nearly eco-friendly pollutant degradation. The findings reveal how to use the Sabatier principle to guide the design of advanced SACs for efficient pollutant removal.