Pyrolyzed iron–nitrogen–carbon hybrids for efficient contaminant decomposition via periodate activation: Active site and degradation mechanism

The practical application of periodate-based advanced oxidation technologies (PI-AOTs) for wastewater treatment requires efficient and cost-effective activators. Pyrolyzed Fe–N/C materials are potential candidates, however, their actual active sites and activation mechanisms are yet to be fully unde...
Ausführliche Beschreibung

The practical application of periodate-based advanced oxidation technologies (PI-AOTs) for wastewater treatment requires efficient and cost-effective activators. Pyrolyzed Fe–N/C materials are potential candidates, however, their actual active sites and activation mechanisms are yet to be fully understood. Herein, a series of Fe–N/C samples (denoted as FeNC-X) with differing structures and iron components were delicately synthesized. Experimental studies on the structure–activity relationship and density functional theory (DFT) computations revealed that Fe–Nx species serve as the dominant active site for periodate activation, while the inactive iron-based particles (i.e., Fe0 and Fe3C) optimized the binding affinity of surrounding carbon layers with periodate, resulting in enhanced activity. In-depth exploration of the oxidative mechanism revealed that Fe@NC-X activated periodate through an electron transfer regime. Our results also showed that the optimal Fe@NC-0.2/periodate system was highly effective in catalyzing the oxidation of 4-CP, outperforming many reported activators. These findings provide an indispensable foundation for the rational development of advanced Fe–N/C activators and offer vital insights into the mechanism underlying pollutant destruction through PI-AOTs. Ausführliche Beschreibung