This study develops a highly efficient Fe/TiO-O single-atom catalyst to explore the synergistic effect in the photo-Fenton mineralization of phenol. Via using diverse in-situ spectroscopies and density functional theory calculations, the catalytic mechanism is unraveled. That is, oxygen vacancies can significantly accelerate photogenerated charge separation and oriented delivery to Fe single atoms for fast generation of reactive oxygen species, as well as promote the selective adsorption/activation of phenol. As a result, the C-H bonds on phenol were deeply oxidized (conversion: > 91%), accompanied by the mineralization of the benzene ring, with CO and HO as end products (mineralization rate: 66%). Such concerted catalysis between Fe single atoms and oxygen vacancies results in a high reactivity for phenol photo-Fenton mineralization, which is superior to most reported transition-metal-based catalysts. Our finding is expected to provide guidance for designing high-efficiency heterogeneous catalysts in the photo-Fenton catalytic process.

中文翻译：

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Fe1/TiO2 单原子催化剂中氧空位依赖性效应对苯酚光芬顿矿化的高度增强的机制洞察


本研究开发了一种高效的Fe/TiO-O单原子催化剂，以探讨苯酚光芬顿矿化中的协同效应。通过使用不同的原位光谱和密度泛函理论计算，催化机制被揭示。也就是说，氧空位可以显着加速光生电荷分离和定向传递到Fe单原子以快速产生活性氧，并促进苯酚的选择性吸附/活化。结果，苯酚上的C-H键被深度氧化（转化率：>91%），并伴随着苯环的矿化，最终产物为CO和H2O（矿化率：66%）。 Fe单原子和氧空位之间的这种协同催化作用导致苯酚光芬顿矿化具有高反应活性，优于大多数报道的过渡金属基催化剂。我们的发现有望为光芬顿催化过程中设计高效多相催化剂提供指导。