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Photocatalytic Molecular Oxygen Activation Over Single-Atom Fe Decorated {001}-Faceted TiO2 Nanosheets for Formaldehyde Degradation
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DOI：10.1002/adsu.70557.png)
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Abstract
En 中文
This study systematically investigated the catalytic oxidation performance of single-atom iron (Fe)-doped titanium dioxide (Fe/TiO2) photocatalysts toward gaseous formaldehyde (HCHO) under visible light irradiation. The experimental results demonstrated that the incorporation of single-atom Fe significantly enhanced the photocatalytic activity, attaining a 99.05% HCHO removal rate (residual concentration of 0.43 ppm after 1 h), outperforming most TiO2-based materials. The fundamental enhancement mechanism was elucidated using in situ DRIFTS spectroscopy, EPR, TOF-SIMS, and DFT calculations. The results revealed that single Fe atoms and oxygen vacancies serve as active sites and electron reservoirs, thereby enhancing molecular oxygen activation by promoting electron transfer to the π-antibonding orbital (π2p*) of O2. Consequently, this process generated highly reactive monoatomic oxygen anions (O−) as the dominant reactive oxygen species. Further mechanistic analysis has confirmed that the O− species can oxidize HCHO through a DOM intermediate pathway, ultimately mineralizing it into CO2 and H2O. This study elucidated the pivotal role of O− radicals in the deep oxidation of HCHO and provided novel theoretical insights and strategic guidance for the design of highly efficient TiO2-based air-purification materials.
Keywords:
HCHO oxidation
monoatomic oxygen ion
oxygen molecule activation
single Fe atom
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