Carbon Nitride Supported High‐Loading Fe Single‐Atom Catalyst for Activation of Peroxymonosulfate to Generate <sup>1</sup>O<sub>2</sub> with 100 % Selectivity
Longshuai Zhang, Xunheng Jiang, Zi‐Ai Zhong, Lei Tian, Qing Sun, Yi‐Tao Cui, Xin Lü, Jian‐Ping Zou, Shenglian Luo
Abstract
Abstract Singlet oxygen ( 1 O 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 1 O 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 % 1 O 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 SO 5 .− , and thereafter efficiently generate 1 O 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 1 O 2 for highly selective and efficient degradation of pollutants.