Boosting Fenton-like reactions via single atom Fe catalysis

Abstract

The maximization of the numbers of exposed active sites in supported metal catalysts is important to achieve high reaction activity. In this work, a simple strategy for anchoring single atom Fe on SBA-15 to expose utmost Fe active sites was proposed. Iron salts were introduced into the as-made SBA-15 containing the template and calcined for simultaneous decomposition of the iron precursor and the template, resulting in single atom Fe sites in the nanopores of SBA-15 catalysts (SAFe-SBA). X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (UV-vis DRS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and extended X-ray absorption fine structure (EXAFS) imply the presence of single atom Fe sites. Furthermore, EXAFS analysis suggests the structure of one Fe center with four O atoms, and density functional theory calculations (DFT) simulate this structure. The catalytic performances of SAFe-SBA were evaluated in Fenton-like catalytic oxidation of p-hydroxybenzoic acid (HBA) and phenol. It was found that the single atom SAFe-SBA catalysts displayed superior catalytic activity to aggregated iron sites (AGFe-SBA) in both HBA and phenol degradation, demonstrating the advantage of SAFe-SBA in catalysis.