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可见光辐照下三维N-TiO2/Ti网状光催化体系降解DMP
引用本文:付亮,贾玉红,尤宏,国谦,李维国.可见光辐照下三维N-TiO2/Ti网状光催化体系降解DMP[J].哈尔滨工业大学学报,2019,51(10):171-177.
作者姓名:付亮  贾玉红  尤宏  国谦  李维国
作者单位:哈尔滨工业大学(威海)海洋科学与技术学院,山东威海,264209;哈尔滨工业大学(威海)海洋科学与技术学院,山东威海264209;城市水资源与水环境国家重点实验室(哈尔滨工业大学),哈尔滨150090
基金项目:城市水资源与水环境国家重点实验室自主课题(2016DX12)
摘    要:为在可见光LEDs(visible light LEDs,vis-LEDs)辐照下实现邻苯二甲酸二甲酯(Dimethyl phthalate,DMP)的有效去除,通过向电解液中加入尿素的一步阳极氧化法在钛网表面制备N-TiO_2/Ti网状光催化剂,并将N-TiO_2/Ti网以多层叠加的方式布置于反应器内对DMP进行降解.采用场发射扫描电子显微镜、能量色散X射线光谱、X射线衍射光谱、X射线光电子能谱以及紫外-可见漫反射吸收光谱等分析方法对N-TiO_2/Ti网进行表征.结果显示:N元素主要以取代氮形态参与到晶格构成中,且未引起TiO_2纳米管的表面形貌和晶型结构改变;由Tauc/David-Mott公式计算得N-TiO_2/Ti网的禁带宽度约为2.76 eV,吸收带边红移至449 nm,可见光吸收性能明显增强.N-TiO_2/Ti板等价拉伸成3层叠加的N-TiO_2/Ti网后,DMP的降解率提高了7.5%;当叠加5层N-TiO_2/Ti网时,降解率趋于稳定,相比N-TiO_2/Ti板对DMP的降解率提升了25.7%;偏酸或偏碱性条件下,均有利于DMP的降解;外加H_2O_2可以明显促进DMP的降解,但H_2O_2在单独使用以及可见光辐照下均无法实现对DMP的有效降解.

关 键 词:三维  氮掺杂  钛网  可见光LED  邻苯二甲酸二甲酯
收稿时间:2018/8/16 0:00:00

Photocatalytic degradation of DMP using 3-D stacked N-TiO2/Ti mesh under visible light
FU Liang,JIA Yuhong,YOU Hong,GUO Qian and LI Weiguo.Photocatalytic degradation of DMP using 3-D stacked N-TiO2/Ti mesh under visible light[J].Journal of Harbin Institute of Technology,2019,51(10):171-177.
Authors:FU Liang  JIA Yuhong  YOU Hong  GUO Qian and LI Weiguo
Affiliation:College of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai 264209, Shandong, China,College of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai 264209, Shandong, China,College of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai 264209, Shandong, China ;State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology, Harbin 150090, China,College of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai 264209, Shandong, China and College of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai 264209, Shandong, China
Abstract:To achieve effective removal of Dimethyl phthalate (DMP) under visible light LED (Vis-LED), N-TiO2/Ti network catalyst was prepared on the surface of titanium mesh by one-step anodic oxidation of adding urea to electrolyte solution, and the DMP was degraded by multiple layers of N-TiO2/Ti mesh superposed in a reactor. The N-TiO2/Ti mesh was characterized by field emission scanning electron microscopy (FESEM), energy dispersive X-ray spectroscopy (EDX), X-ray diffraction spectroscopy (XRD), X-ray photoelectron spectroscopy (XPS), and UV-visible diffuse reflectance spectroscopy (UV-vis DRS). Results show that N element mainly participated in the form of substituted nitrogen, and both surface morphology and crystal structure of the TiO2 nanotubes were not changed. The forbidden band width of the N-TiO2/Ti mesh calculated by the Tauc/David-Mott formula was about 2.76 eV, and the absorption band edge was extended to 449 nm, where the visible light absorption performance was significantly enhanced. After the N-TiO2/Ti foil was equivalently stretched into 3 layers of N-TiO2/Ti mesh, the degradation rate of DMP increased by 7.5%. When 5 layers of N-TiO2/Ti mesh were superposed, the degradation rate of DMP tended to be stable and it increased by 25.7% compared with that of Ni-TiO2/Ti plate. Partial acidity or alkaline was beneficial to the degradation of DMP. The addition of H2O2 could promote the degradation of DMP, but H2O2 could not effectively degrade DMP under single use and visible light irradiation.
Keywords:3-D  nitrogen-doped  Ti mesh  visible light LED  Dimethyl phthalate
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