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

Abstract

Singlet oxygen (1O2) 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 1O2. 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 % 1O2 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 1O2 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 1O2 for highly selective and efficient degradation of pollutants.

Research Progress and Application of Single-Atom Catalysts: A Review

“…When the size of nanocrystal is reduced to the form of clusters of atoms and single atoms, its energy level structure and electronic structure will also be completely changed. Because of its unique structural characteristics, single-atom catalysts show higher activity, stability, and selectivity than traditional nanocatalysts, and efficiently promote the progress of catalytic reactions [18].…”

0D–1D hybrid nanoarchitectonics: tailored design of FeCo@N–C yolk–shell nanoreactors with dual sites for excellent Fenton-like catalysis

“…2c ) displays a peak at 1.7 Å, which is ascribed to the Fe–N bond, and a remarkable peak at approximately 2.25 Å corresponding to the metal–metal band. 10,30 The Co K-edge and EXAFS spectra (Fig. S6 † ) also confirm the presence of Co–N and the metal–metal band.…”

“… 5–9 Over the past two decades, heterogeneous catalysis has emerged as the most effective approach to water treatment, with much effort dedicated to developing better catalysts, including transition metal-based and carbonaceous materials. 10,11 Unfortunately, most metal-based catalysts suffer from leaching of toxic metal ions, which can thwart their practical application, 12,13 and although carbonaceous catalysts produce no secondary pollution, their cycle performance is always depressed. 14 There is therefore an urgent need to find robust catalysts with adequate activity and stability for Fenton-like processes.…”

Nanoscale Self‐Wetting Driven Monatomization of Ag Nanoparticle for Excellent Photocatalytic Hydrogen Evolution

“…In further, the origin of excellent photocatalytic HER activity of SACs has been studied widely. [47][48][49][50] The SACs usually own extremely high ratio of exposed atoms and high atomic utilization efficiency. The superior photocatalytic HER performance of Ag 1 /CN than Ag NPs/CN stem from more visible light absorbtion ability, suitable electronic structure and hydrogen and the high atomic utilization efficiency.…”