School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China; State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China; Key Laboratory of advanced catalysis, Gansu Province, State Key Laboratory of Applied Organic Chemistry College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China.
Water Res. 2024 Sep 15;262:122101. doi: 10.1016/j.watres.2024.122101. Epub 2024 Jul 15.
Fluorinated pharmaceuticals pollution has become an ever-increasing environmental concern due to its negative impacts. Photoelectrocatalytic (PEC) degradation system is a desirable approach to tackle the pollution problems. However, photogenerated charge separation and interfacial mass transfer are the main bottlenecks for improving the PEC degradation performance. Herein, we report a TiO photoanode with tuned (101)/(110) facets in situ grown on a Ti mesh substrate for PEC degradation of fluorinated pharmaceuticals. The exposure of (101) facets facilitates efficient photogenerated charge separation and the desorption of generated •OH radical. Besides, the three-dimensional (3D) architecture of photoanode promotes macroscopic mass transfer. This system performed complete defluorination of 5-fluorouracil and more than 75 % total organic carbon (TOC) removal efficiency. The apparent reaction rate constant of high (101) facet-exposed TiO grown on Ti mesh is up to 6.96 h, 6‒fold faster than that of photoanode with low (101) facet-exposed TiO grown on Ti foil. It is demonstrated that a large-sized PEC system of 1200 cm can degrade 100 L of synthetic fluorinated pharmaceutical wastewater with more than 80 % elimination efficiency. This work showcases the facet and substrate modulated strategy of fabricating high-performed photoanode for PEC wastewater purification.
由于氟代药物的负面影响，其污染已成为日益严重的环境问题。光电催化（PEC）降解系统是解决污染问题的一种理想方法。然而，光生电荷分离和界面传质是提高 PEC 降解性能的主要瓶颈。在此，我们报告了一种在 Ti 网基底上原位生长的具有可调（101）/（110）晶面的 TiO 光阳极，用于 PEC 降解氟代药物。（101）晶面的暴露有利于光生电荷的有效分离和生成的 •OH 自由基的解吸。此外，光阳极的三维（3D）结构促进了宏观传质。该体系可完全脱氟 5-氟尿嘧啶，TOC 去除率超过 75%。在 Ti 网上生长的具有高（101）晶面暴露的 TiO 的表观反应速率常数高达 6.96 h-1，比在 Ti 箔上生长的具有低（101）晶面暴露的光阳极快 6 倍。实验证明，一个 1200 cm2 的大型 PEC 系统可以降解 100 L 的合成氟代药物废水，去除率超过 80%。这项工作展示了用于 PEC 废水净化的具有高性能光阳极的晶面和基底调制策略。
