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.
Keywords: coordination environment; peroxymonosulfate; sabatier principle; singlet oxygen; single‐atom catalysts.
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