Boosting Reactive Oxygen Species Generation via Contact‐Electro‐Catalysis with FeIII‐Initiated Self‐cycled Fenton System

Abstract Contact Electro‐Catalysis (CEC) using commercial dielectric materials in contact‐separation cycles with water can trigger interfacial electron transfer and induce the generation of reactive oxygen species (ROS). However, the inherent hydrophobicity of commercial dielectric materials limits the effective reaction sites, and the generated ROS inevitably undergo self‐combination to form hydrogen peroxide (H 2 O 2 ). In typical CEC systems, H 2 O 2 does not further decompose into ROS, leading to suboptimal reaction rates. Addressing the generation and activation of H 2 O 2 is therefore crucial for advancing CEC. Here, we synthesized a catalyst by loading the dielectric material polytetrafluoroethylene (PTFE) onto ZSM‐5 (PTFE/ZSM‐5, PZ for short), achieving uniform dispersion of the catalyst in water for the first time. The introduction of an Fe III ‐initiated self‐cycling Fenton system (SF‐CEC), with the synergistic effects of O 2 activation and Fe III ‐activated H 2 O 2 , further enhanced ROS generation. In the Fe III ‐initiated SF‐CEC system, the synergistic effects of ROS and protonated azo dyes enabled nearly 99 % degradation of azo dyes within 10 minutes, a sixfold improvement compared to the CEC system. This represents the fastest degradation rate of methyl orange dye induced by ultrasound to date. Without extra oxidants, this system enabled stable dissolution of precious metals in weakly acidic solutions at room temperature, achieving 80 % gold dissolution within 2 hours, 2.5 times faster than similar CEC systems. This study also corrects the unfavorable perception of CEC applications under acidic conditions, providing new insights for the fields of dye degradation and precious metal recovery.