Enhanced Fenton-like catalysis via interfacial regulation of g-C3N4 for efficient aromatic organic pollutant degradation.

For the efficient degradation of organic pollutants with the goal of reducing the water environment pollution, we employed an alkaline hydrothermal treatment on primeval g-C 3 N 4 to synthesize a hydroxyl-grafted g-C 3 N 4 (CN-0.5) material, from which we engineered a novel Fenton-like catalyst, known as Cu–CN-0.5. The introduction of numerous hydroxyl functional groups allowed the CN-0.5 substrate to stably fix active copper oxide particles through surface complexation, resulting in a low Cu leaching rate during a Cu–CN-0.5 Fenton-like process. A sequence of characterization techniques and theoretical calculations uncovered that interfacial complexation induced charge redistribution on the Cu–CN-0.5 surface. Specifically, some of the π electrons in the tris-s-triazine units were transferred to the copper oxide particles along the newly formed chemical bonds (C (π) -O-Cu), forming a π-deficient area on the tris-s-triazine plane near the complexation site. In a typical Cu–CN-0.5 Fenton-like process, a stable π-π interaction was established due to the favorable positive-negative match of electrostatic potential between the aromatic pollutants and π-deficient areas, leading to a significant improvement in Cu–CN-0.5's adsorption capacity for aromatic pollutants. Furthermore, pollutants also delivered electrons to the Cu–CN-0.5 Fenton-like system via a "through-space" approach, which suppressed the futile oxidation of H 2 O 2 in reducing the high-valent Cu²⁺ and significantly improved the generation efficiency of ^•OH with high oxidative capacity. As expected, Cu–CN-0.5 not only exhibited an efficient Fenton degradation for several typical aromatic organic pollutants, but also demonstrated both a low metal leaching rate (0.12 mg/L) and a H 2 O 2 utilization rate exceeding 80%. The distinctive Fenton degradation mechanism substantiated the potential of the as-prepared material for effective wastewater treatment applications. [Display omitted] • A unique interfacial regulation strategy for Enhancing Fenton activity. • Effective adsorption of pollutants by Fenton catalyst achieved through π-π Stacking. • Expanding novel theoretical computational methods to Fenton reaction domain. • The system significantly improved the H 2 O 2 utilization and the.^•OH generation efficiency. [ABSTRACT FROM AUTHOR]