Mesoporous structure and amorphous Fe-N sites regulation in Fe-g-C3N4 for boosted visible-light-driven photo-Fenton reaction
| Autor: | Shifei Kang, Lulu Zheng, Lifeng Cui, Chenjie Ding, Weikang Gao, Wenxin Li, Zhihao Zhang |
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| Rok vydání: | 2022 |
| Předmět: |
Materials science
Metal ions in aqueous solution Crystal structure Surfaces Coatings and Films Electronic Optical and Magnetic Materials Catalysis Biomaterials Metal Colloid and Surface Chemistry Chemical engineering Chemical bond Polymerization visual_art visual_art.visual_art_medium Mesoporous material Visible spectrum |
| Zdroj: | Journal of Colloid and Interface Science. 608:2515-2528 |
| ISSN: | 0021-9797 |
| Popis: | Heterogeneous photo-Fenton catalysts prepared by doping metal ions in g-C3N4 are promising alternatives to traditional homogeneous Fenton catalysts, but are restricted by poor mesoporous structure and agglomerate of metal species. Recently, the highly uniformly dispersed metal-N active sites in various photocatalysts have been proved to be the critical reason for their enhanced catalytic activity. In this study based on reasonable control of mesoporous structure and metal-N active sites, mesoporous Fe-g-C3N4 was synthesized using a simple one-step thermal shrinkage polymerization method using ferrous oxalate as iron source and pore-forming agent. The Fe and N elements in the triazine ring skeleton of Fe-g-C3N4 form a σ-π bond, thus the photogenerated electrons can be quickly transferred to Fe3+ to form Fe2+ under the interaction of chemical bonds, accelerating the Fenton reaction rate. Density functional theory calculations results demonstrate that the energy band structure and electron cloud density distribution of Fe-Nx active structure are better than that of routine FeOx crystal structure with metal species agglomeration. In addition, the excellent mesoporous structure of Fe-g-C3N4 creates conditions for the high exposure of Fe-Nx active sites in the photo-Fenton reaction under visible light. The as-developed Fe-g-C3N4 system shows high recyclability and excellent photo-Fenton performance for removal of typical intractable pollutants (The degradation rate of dye and tetracycline reaches 98.2% and 98.7% at 60 and 120 min, respectively). This work provides a facile and sustainable route to develop mesoporous highly-active heterogeneous Fenton-like catalysts and even further general the design of general catalyst with ideal metal-N active sites, thereby promoting a feasible and efficient wastewater remediation solution. |
| Databáze: | OpenAIRE |
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