Insight into the role of heterogeneous Fenton-like catalyst FeCo-γ-Al2O3 with dual electron-rich centers for Ni-EDTA removal

Abstract

To enhance the polarization distribution of electron cloud density on the catalyst surface, we have introduced a novel bimetallic-substituted dual-reaction center (DRC) catalyst (FeCo-γ-Al₂O₃) comprising iron (Fe) and cobalt (Co) for the decomplexation and mineralization of heavy metal complex Ni-EDTA in this study. Compared to the catalysts doped solely with Fe or Co, the bimetal-doped catalyst offered several advantages, including enhanced electron cloud polarization distribution, additional electron transfer pathway, and improved capacity of free radical generation. Through DFT calculations and EPR tests, we have elucidated the influences of the catalyst's adsorption toward Ni-EDTA and its decomplexation products on the electron transfer between the pollutant and the catalyst. The competition between the pollutants and H₂O₂ affects the generation of free radicals in both electron-rich Fe and Co centers as well as electron-deficient Al center. Building on these findings, we have proposed a plausible removal mechanism of Ni-EDTA using the heterogeneous Fenton-like catalyst FeCo-γ-Al₂O₃. This study sheds light on the potential of FeCo-γ-Al₂O₃ as a DRC catalyst and emphasizes the significance of pollutant characteristics in determining the catalyst's performance.

Keywords: Density functional calculation; Dual electron-rich centers; Heavy metal complex; Heterogeneous fenton-like catalyst; Reaction mechanism.