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

Singlet oxygen (O-1(2)) 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 O-1(2). In this work, we develop a graphitic carbon nitride supported Fe single-atoms catalyst (Fe-1/CN) containing highly uniform Fe-N-4 active sites with a high Fe loading of 11.2 wt %. The Fe-1/CN achieves generation of 100 % O-1(2) 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-N-4 sites in Fe-1/CN adsorb the terminal O of PMS, which can facilitate the oxidization of PMS to form SO5.-, and thereafter efficiently generate O-1(2) with 100 % selectivity. In addition, the Fe-1/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 O-1(2) for highly selective and efficient degradation of pollutants.

Automated summary

A novel catalyst Fe-1/CN was developed to achieve 100% selective production of O-1(2) through activation of PMS, enabling highly selective and efficient degradation of organic pollutants.