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Mechanisim investigation on the enhanced and selective photoelectrochemical oxidation of atrazine on molecular imprinted mesoporous TiO2

DOI:10.1016/j.apcatb.2019.01.018 期刊:Applied Catalysis B: Environmental 出版年份:2019 更新时间:2025-09-23 15:22:29
摘要: In this work, enhanced and selective photoelectrochemical (PEC) oxidation of atrazine was realized on molecular imprinted mesoporous TiO2 (MI-meso-TiO2). The investigation revealed that, for one hand, the surface MI sites could function as surface defects for accelerating the separation of photogenerated holes and electrons, leading to enhanced generation of hydroxyl radicals. For the other hand, the MI sites showed enhanced binding affinity toward atrazine, resulted from the formation of multiple hydrogen bonds and halogen bonds etc., which was testified by in situ ATR-FTIR spectra. It led to the enhanced adsorption and improved local concentration of atrazine on the electrode surface. Both the two factors contributed to the improved PEC oxidation activity for atrazine on MI-meso-TiO2 compared with that on meso-TiO2. Moreover, the high binding affinity between MI sites and atrazine resulted in the selective recognition ability toward atrazine in the presence of the coexisting pollutants, so that selective PEC oxidation of atrazine in complex polluted water samples was successfully achieved on MI-meso-TiO2 with the apparent rate constant of 0.25 h-1, whereas that on meso-TiO2 was only 0.08 h-1. This work provided something new for explaining the selective and enhanced PEC performance on molecular imprinting catalyst.
作者: Huijie Shi,Yingling Wang,Chunjing Tang,Weikang Wang,Meichuan Liu,Guohua Zhao
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To investigate the mechanism behind the enhanced and selective photoelectrochemical oxidation of atrazine using molecular imprinted mesoporous TiO2, focusing on the roles of MI sites in improving charge transfer, hydroxyl radical generation, and binding affinity for selective recognition in complex water samples.

MI-meso-TiO2 significantly enhances PEC oxidation of atrazine through improved charge transfer, increased hydroxyl radical generation, and strong binding affinity due to multiple supramolecular interactions. It demonstrates selective recognition in complex water, with higher efficiency and lower activation energy compared to non-imprinted TiO2, offering a promising approach for targeted water treatment.

The study is limited to atrazine and a few similar compounds; the stability and scalability of MI-meso-TiO2 for industrial applications are not fully explored. Potential optimizations include testing with a wider range of pollutants and under varying environmental conditions.

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