Polypyrrole-decorated resorcinol-formaldehyde microspheres for sustainable in-situ H2O2 photocatalytic generation and eco-friendly pollutant removal.

The development of sustainable and efficient systems for the complete degradation of organic pollutants under mild conditions remains a major environmental challenge. Conventional Fenton systems often rely on externally supplied H2O2, which introduces storage and transport risks as well as additional operational costs. In this work, a polypyrrole-decorated resorcinol-formaldehyde microsphere (PPy/RF) photocatalyst was rationally constructed via in-situ oxidative polymerization to integrate photocatalytic H2O2 generation and photo-Fenton oxidation within a single platform. The donor-acceptor (D-A) interfacial structure formed between PPy and RF effectively broadens visible-light absorption, accelerates charge transfer, and facilitates efficient in-situ H2O2 formation. More importantly, the generated H2O2 directly participates in the photo-Fenton process with Fe3+/Fe2+ redox cycling, leading to the continuous generation of highly reactive hydroxyl radicals (·OH) and superoxide radicals (·O2-). Under visible-light irradiation, the optimized PPy/RF-0.07 exhibited a markedly enhanced H2O2 production rate (727.56 μM h-1) due to the D-A interfacial structure between RF and PPy promotes oxygen reduction reaction (ORR) and water oxidation reaction (WOR). Subsequently, it achieved an outstanding degradation efficiency (>99%) toward phenol, dyes, and antibiotics, outperforming conventional systems that require external H2O2 dosing. This superior performance originates from the synergistic effects of enhanced interfacial charge separation, in-situ H2O2 self-supply, and photo-Fenton-driven radical oxidation. This work demonstrates a self-sustaining photo-Fenton-like system that eliminates the dependence on external oxidants, offering a new insight for solar-driven advanced oxidation processes and sustainable wastewater treatment.