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

Abstract 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‐N 2 O 2 /C catalyst demonstrates a degradation rate constant of 1.89 min −1 , surpassing Fe‐N 4 /C by 3.2 times and Fe‐O 4 /C by 272 times. Moreover, Fe‐N 2 O 2 /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.