The degradation mechanism study of 17α-ethinylestradiol by TiO2 nanobelt/pg-C3N4 photocatalyst under visible light irradiation
LUO Li-jun1, MENG De-mei1, DAI Jian-hui1, LI Jun-Hong1, ZHENG Li-bo1, XIA Li-hong1, JIANG Feng-zhi2
1. Key Laboratory of Green-Chemistry Materials in University of Yunnan Province, School of Chemistry and Environment, Yunnan Minzu University, Kunming 650500, China; 2. Key Laboratory of Medicinal Chemistry for Natural Resource, Ministry of Education, Yunnan University, Kunming 650091, China
Abstract：TiO2-NB/pg-C3N4 photocatalysts were prepared using prepared porous C3N4 nanosheets and TiO2 nanobelts via grinding and followed calcination, and the preparation conditions were optimized. The prepared materials were used to remove 17α-ethynylestradiol(EE2) under visible light irradiation, which has most potent estrogenic activity. The structure and surface physical-chemical properties of them were comprehensively investigated by scanning electron microscope (SEM), transmission electron microscopy (TEM), x-ray diffraction (XRD), ultraviolet visible diffuse reflectance spectroscopy (UV-Vis DRS), photoluminescence spectroscopy (PL), X-ray photoelectron spectroscopy (XPS) and N2 adsorption-desorption isotherms (BET). The results showed that the B-type TiO2 nanobelts were anchored onto porous C3N4 nanosheets to form TiO2-NB/pg-C3N4 composite photocatalyst. The degradation rate constants of EE2 on TiO2-NB/pg-C3N4 (0.02537min-1) was 12.88 times and 3.29 times than those on pure TiO2-NB(0.00197min-1) and pg-C3N4(0.0077min-1). Active species capture experiments showed that ·O2- was the main active specie in the EE2 degradation process on TiO2-NB/pg-C3N4. The HPLC-high resolution mass spectrum (HPLC-HRMS) measurement results showed that there were 4 intermediates and possible degradation route was proposed. Moreover, the estrogenic activity measurement by MCF-7method during degradation process showed that TiO2-NB/pg-C3N4 can effectively eliminate the estrogenic activity without producing by-products with more estrogenic activity.
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