The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 2, 2024

The photoaccelerated Fenton reaction on semiconductors has gained increasing attention for wastewater treatment, with FeOCl showing superior OH• radical generation. However, the atomic-level mechanism behind this enhanced activity remains unclear. In study, we performed first-principles calculations to compare photo-Fenton FeOCl(100) under photocatalytic and thermocatalytic conditions. Our results identify [Fe2+–Fe3+] unit as key active site driving reaction. Fe2+ promotes cleavage of O–O bond in H2O2 generate radical, while Fe3+ aids desorption OH•. Under conditions, from rapid Fe2+/Fe3+ cycling driven by a photogenerated electron. contrast, thermocatalysis relies additional reduce Fe2+. Although holes can also contribute trapping OH– form their effect is relatively secondary due lower hole-trapping capacity surface compared electron trapping. A comparison Fe2O3(012) catalyst reveals that both promote photoirradiation, suffers stronger OH binding its higher donation capacity. addition, V-shaped structure bidentate adsorption, intensifying excessive adsorption intermediates limiting desorption. FeOCl's moderate contributes catalytic efficiency. This study provides insights into mechanism, highlighting role light, offers guidance designing more effective catalysts comparing Fe2O3.

Language: Английский