Carbon-driven advanced oxidations show great potential in water purification, but regulating structures and properties of carbon-based catalysts to achieve ultrafast Fenton-like reactions remains challenging. Herein, a biomorphic diatomite-based catalyst (BD-C) with Si-O doping was prepared using natural diatomite as silicon source and porous template. The results showed that the metal-free BD-C catalyst exhibited ultrafast oxidation performances (0.95-2.58 min-1) towards a variety of pollutants in PMS-based Fenton-like reaction, with the Fenton-like activity of metal-free catalyst comparable to metal-based catalysts or even single-atom catalysts. Pollutants (e.g., CP, BPA, TC, and PCM) with electron-donating groups exhibited extremely low PMS decomposition with overwhelmed electron transfer process (ETP), while high PMS consumption was induced by the addition of electron-withdrawing pollutants (e.g., MNZ and ATZ), which was dominated by radical oxidation. The BD-C/PMS system also showed a high ability to resist the environmental interference. In-depth theoretical investigations demonstrated that the coordination of Si-O can lower the potential barrier of PMS activation for accelerating the generation of radicals, and also promote the electron transfer from pollutants to the BD-C/PMS complexes. In addition, BD-C was deposited onto a polytetrafluoroethylene membrane (PTFEM) with 100% of pollutants removal over 10 h, thereby revealing the promising prospects of utilizing BD-C for practical applications.
Keywords: Diatomite; Electron transfer process (ETP); Fenton-like reaction; Peroxymonosulfate; Si–O doping.
Copyright © 2024 Elsevier Ltd. All rights reserved.