通过铁基高级氧化过程（AOPs）实现快速连续产生活性氧（ROS）在环境和生物领域具有重要意义。然而，目前由助催化剂辅助的AOP仍然存在质量/电子转移差和不持久的促进作用，导致Fe²⁺/Fe³⁺循环缓慢，ROS产生的Fe²⁺动态浓度低。在此，我们提出了一种用二硫化钼（MoS₂）官能化的三维（3D）宏观助催化剂，通过循环流通过程实现了超高效的Fe²⁺再生（平衡Fe²⁺比为82.4%）和显著的稳定性（超过20个循环）。与传统的间歇式反应器不同，实验和计算流体动力学模拟表明，在流通模式下，由对流增强的质量/电荷转移引发的Fe²⁺还原，然后由MoS₂诱导的流动旋转加强，以实现充分的反应物混合，对氧化剂活化和随后的ROS生成至关重要。引人注目的是，具有超润湿能力的流通共催化系统甚至可以处理由不同表面活性剂稳定的复杂含油废水，而不会损失污染物降解效率。我们的研究结果强调了一种创新的助催化剂系统设计，以扩大基于AOP的技术的适用性，特别是在大规模复杂的废水处理中。

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 Fe²⁺/Fe³⁺ cycle and low dynamic concentration of Fe²⁺ for ROS production. Herein, we present a three-dimensional (3D) macroscale co-catalyst functionalized with molybdenum disulfide (MoS₂) to achieve ultra-efficient Fe²⁺ regeneration (equilibrium Fe²⁺ 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 Fe²⁺ reduction and then strengthened by MoS₂-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.