Carbon Nitride Supported High‐Loading Fe Single‐Atom Catalyst for Activation of Peroxymonosulfate to Generate 1O2 with 100 % Selectivity

Singlet oxygen (¹ O₂ ) is an excellent active species for the selective degradation of organic pollutions. However, it is difficult to achieve high efficiency and selectivity for the generation of ¹ O₂ . In this work, we develop a graphitic carbon nitride supported Fe single-atoms catalyst (Fe₁ /CN) containing highly uniform Fe-N₄ active sites with a high Fe loading of 11.2 wt %. The Fe₁ /CN achieves generation of 100 % ¹ O₂ by activating peroxymonosulfate (PMS), which shows an ultrahigh p-chlorophenol degradation efficiency. Density functional theory calculations results demonstrate that in contrast to Co and Ni single-atom sites, the Fe-N₄ sites in Fe₁ /CN adsorb the terminal O of PMS, which can facilitate the oxidization of PMS to form SO₅ ^.- , and thereafter efficiently generate ¹ O₂ with 100 % selectivity. In addition, the Fe₁ /CN exhibits strong resistance to inorganic ions, natural organic matter, and pH value during the degradation of organic pollutants in the presence of PMS. This work develops a novel catalyst for the 100 % selective production of ¹ O₂ for highly selective and efficient degradation of pollutants.