Mass Transfer-Promoted Fe2+/Fe3+ Circulation Steered by 3D Flow-Through Co-Catalyst System Toward Sustainable Advanced Oxidation Processes

Realizing fast and continuous generation of reactive oxygen species (ROSs) via iron-based advanced oxidation processes (AOPs) is significant in the environmental and biological fields. However, current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect, giving rise to the sluggish Fe 2+ /Fe 3+ cycle and low dynamic concentration of Fe 2+ for ROS production. Herein, we present a three-dimensional (3D) macroscale co-catalyst functionalized with MoS 2 to achieve ultra-efficient Fe 2+ regeneration (equilibrium Fe 2+ ratio of 82.4%) and remarkable stability (more than 20 cycles) via a circulating flow-through process. Unlike the conventional batch-type reactor, experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode, initiated by the convection-enhanced mass/charge transfer for Fe 2+ reduction and then strengthened by MoS 2 -induced flow rotation for sufficient reactant mixing, is crucial for oxidant activation and subsequent ROS generation. Strikingly, the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency. Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology, especially in large-scale complex wastewater treatment.