As highly active species, in theory, hydroxyl radicals (OH) can move freely and destroy almost all organic compounds, including catalysts with a conjugate structure. Therefore, a system that can generate oxidative species with a high activity, but where the active species is anchored to avoid autooxidation, is urgently required. In this work, we fabricated a novel visible-light-assisted advanced oxidation process based on high-valent iron species (Fe(IV)O) over graphitic carbon nitride (g-C₃N₄) that was coordinated to iron hexadecachlorophthalocyanine (FePcCl₁₆) through imidazole ligands (IMD). Under visible-light excitation, the phthalocyanine ring of the g-C₃N₄-IMD-FePcCl₁₆/hydrogen peroxide (H₂O₂) can be motivated to an excited state FePcCl₁₆^∗, in which active H₂O₂ and the generation of anchored Fe(IV)O species are used for the degradation of carbamazepine (CBZ). Because the molecular movement of transient Fe(IV)O species is restricted, the possibility of oxidative collision is minimized, which provides good stability. An analysis of the electron paramagnetic resonance, gas chromatography/mass spectrometry, photoluminescence spectra, periodic on/off photocurrent density response and the photo-assisted catalytic active experiments, indicates that the rapid generation of Fe(IV)O species occurs as the catalyst contacts the H₂O₂, which inhibits the conduction-band electrons of the g-C₃N₄ from reacting with H₂O₂ and generating OH. This study provides insight into the construction of suitable structures that will enhance visible-light-assisted catalytic oxidation activity and allow for the fabrication of an anchored highly active species.

从理论上讲，作为高活性物种，羟基自由基（OH）可以自由移动并破坏几乎所有有机化合物，包括具有共轭结构的催化剂。因此，迫切需要一种系统，该系统可以产生具有高活性的氧化物质，但是其中的活性物质被锚定以避免自氧化。在这项工作中，我们制造了一种新型的可见光辅助高级氧化工艺，该工艺基于与十六碳萘酞菁铁（FePcCl ₁₆）配位的石墨氮化碳（gC ₃ N ₄）上的高价铁物种（Fe（IV）O ）。通过咪唑配体（IMD）。在可见光激发下，gC ₃ N ₄ -IMD-FePcCl的酞菁环₁₆ /过氧化氢（H ₂ O ₂）可以被激发为FePcCl ₁₆ ^∗激发态，其中活性H ₂ O ₂和锚定的Fe（IV）O物种的产生被用于卡马西平（CBZ）的降解。由于瞬态Fe（IV）O物种的分子运动受到限制，因此氧化碰撞的可能性降到了最低，从而提供了良好的稳定性。对电子顺磁共振，气相色谱/质谱，光致发光光谱，周期性开/关光电流密度响应和光辅助催化活性实验的分析表明，Fe（IV）的快速生成当催化剂接触H ₂ O ₂时会发生O物种，这会抑制gC ₃ N ₄的导带电子与H ₂ O ₂反应并生成OH。这项研究为构建合适的结构提供了见识，这些结构将增强可见光辅助的催化氧化活性，并允许制造锚定的高活性物种。