Bo Longli, He Kebo, Tan Na, Gao Bo, Feng Qiqi, Liu Jiadong, Wang Lei
School of Environmental and Municipal Engineering, Xi'an University of Architecture and Technology, Yan Ta Road No. 13, Xi'an, 710055, China.
School of Environmental and Municipal Engineering, Xi'an University of Architecture and Technology, Yan Ta Road No. 13, Xi'an, 710055, China.
J Environ Manage. 2017 Apr 1;190:259-265. doi: 10.1016/j.jenvman.2016.12.050. Epub 2017 Jan 4.
In this work, visible-light-driven ZnlnS photocatalyst (band gap 1.98 eV, absorption wavelength 300-600 nm) was synthesized by a facile hydrothermal method for photocatalytic degradation of trace pharmaceutical carbamazepine (CBZ) in aqueous solution, and characterized by UV-Vis diffusive reflectance spectroscopy, BET, SEM and XRD, respectively. It demonstrated that a complete degradation of CBZ was achieved with an optimal ZnlnS dosage of 30 mg/L under a 100 W iodine-gallium lamp irradiation of 20 min, which afforded the reaction rate constant and half-life being respectively 10.44 times higher and 1/8 less than that obtained by a direct photolysis without ZnlnS photocatalyst. A negligible influence of initial solution pH on photocatalytic degradation of CBZ was confirmed under the given pH range of 5.0-9.0. The degradation efficiency of CBZ was slightly decreased from 91% to 84% after five consecutive cycles. Hydroxy radical (·OH) plays an important role in CBZ degradation accompanying a synergistic effect of photogenerated hole (h) and O active species during reaction. Further, 44 intermediates were detected by LCMS-IT-TOF technique and tentative degrading pathways were proposed on the basis of the experimental results.
在本工作中,通过简便的水热法合成了可见光驱动的ZnlnS光催化剂(带隙1.98 eV,吸收波长300 - 600 nm),用于光催化降解水溶液中的痕量药物卡马西平(CBZ),并分别通过紫外可见漫反射光谱、BET、扫描电子显微镜和X射线衍射对其进行了表征。结果表明,在100 W碘镓灯照射20 min的条件下,当ZnlnS的最佳用量为30 mg/L时,CBZ实现了完全降解,其反应速率常数和半衰期分别比无ZnlnS光催化剂的直接光解高出10.44倍和减少至1/8。在5.0 - 9.0的给定pH范围内,初始溶液pH对CBZ光催化降解的影响可忽略不计。连续五个循环后,CBZ的降解效率从91%略有下降至84%。羟基自由基(·OH)在CBZ降解过程中起重要作用,反应过程中光生空穴(h)和O活性物种具有协同效应。此外,通过LCMS - IT - TOF技术检测到44种中间体,并根据实验结果提出了初步的降解途径。