Plant Polyphenol-Driven Polymerization-Confinement Strategy toward Ultrahighly Loaded Atomically Dispersed FeCo Bimetallic Catalysts for Singlet Oxygen-Dominated Fenton-like Reactions

Abstract

Recent progress has brought carbon-confined transition metal catalysts to the forefront as effective agents for Fenton-like reactions. However, achieving a stable integration of densely loaded and well-dispersed transition metals onto carbon support poses significant challenges. Herein, we introduce a plant polyphenol-driven polymerization-confinement method for the synthesis of a highly dispersed FeCo bimetallic catalyst (FeCo@NGB). Utilizing the chelating effect of tea polyphenols with metal ions and their subsequent polymerization and confinement offers a durable solution for stabilizing the FeCo bimetallic sites. The resulting FeCo@NGB demonstrates exceptional performance in activating peroxymonosulfate (PMS) for the swift degradation of tetracycline (TC), with a 99.5% reduction achieved in just 30 min, predominantly through a singlet oxygen (¹O₂)-driven pathway. Experimental and theoretical calculations highlight the pivotal role of atomically dispersed FeN₄–CoN₃ sites in facilitating rapid electron transfer between the catalyst and PMS, thereby enhancing ¹O₂ production. This work not only advances the development of high-performance multiphase catalysts but also introduces a compelling strategy for water purification leveraging nonradical oxidative pathways.