Yang Shaogui, Fu Hongbo, Sun Cheng, Gao Zhanqi
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210093, PR China.
J Hazard Mater. 2009 Jan 30;161(2-3):1281-7. doi: 10.1016/j.jhazmat.2008.04.107. Epub 2008 May 3.
A novel photocatalysis material, F-Si-comodified TiO(2) (FST) powder, was synthesized by ultrasound-assisted hydrolysis. The prepared material was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and UV-visible absorption spectroscopy, respectively. XRD analysis indicated that the phase of FST was pure anatase and Si atoms suppressed the growth of titania crystalline, XPS spectra showed that FST was composed of Ti, O, Si and F element, the band gap energy of FST calculated according to the spectrum of UV-vis absorption was 3.26 eV. The electron spin resonance (ESR) spin-trapping technique using 5,5-dimethyl-1-pyrroline-N-oxide (DMPO) as the spin-trap reagent has been applied to detect free radical intermediates generated from FST. ESR results showed the concentration of the active species (OH) on FST is higher than those on F-doping TiO(2) (FT), Si-modifying TiO(2) (ST) and P25 titania. The degradation of pentachlorophenol (PCP) in the microwave-assisted photocatalysis (MAPC) process was faster than other processes including microwave-assisted direct photolysis (MADP), microwave process alone (MP) and dark process (DP). The photocatalytic activity of FST is much higher than that of ST, FT and P25 titania. It may be attributed to its strong capacity of absorption to the UV-vis irradiation and more hydroxyl radical on surface of FST. In MPAC process, 40 mg L(-1) PCP was completely degraded in 20 min and its corresponding mineralization efficiency was 71%, the pH of solutions decreased from 10.3 to 6.47 and the dechlorination was completed in 12 min. The intermediates products of PCP in MAPC process identified by GC/MS were trichlorophenols (TCP), tetrachlorophenols (TTCP) and tetrachlorocatechol (TTCC) and the possible mechanism of PCP degradation is proposed.
通过超声辅助水解合成了一种新型光催化材料F-Si共改性TiO₂(FST)粉末。分别采用X射线衍射(XRD)、X射线光电子能谱(XPS)和紫外可见吸收光谱对所制备的材料进行了表征。XRD分析表明,FST的相为纯锐钛矿型,Si原子抑制了二氧化钛晶体的生长;XPS光谱表明,FST由Ti、O、Si和F元素组成,根据紫外可见吸收光谱计算得到FST的带隙能量为3.26 eV。采用以5,5-二甲基-1-吡咯啉-N-氧化物(DMPO)为自旋捕获剂的电子自旋共振(ESR)自旋捕获技术检测了FST产生的自由基中间体。ESR结果表明,FST上活性物种(·OH)的浓度高于F掺杂TiO₂(FT)、Si改性TiO₂(ST)和P25二氧化钛上的活性物种浓度。在微波辅助光催化(MAPC)过程中,五氯苯酚(PCP)的降解速度比其他过程更快,包括微波辅助直接光解(MADP)、单独微波过程(MP)和黑暗过程(DP)。FST的光催化活性远高于ST、FT和P25二氧化钛。这可能归因于其对紫外可见辐射的强吸收能力以及FST表面更多的羟基自由基。在MPAC过程中,40 mg L⁻¹的PCP在20分钟内完全降解,其相应的矿化效率为71%,溶液的pH值从10.3降至6.47,脱氯在12分钟内完成。通过气相色谱/质谱(GC/MS)鉴定了MAPC过程中PCP的中间产物为三氯苯酚(TCP)、四氯苯酚(TTCP)和四氯邻苯二酚(TTCC),并提出了PCP降解的可能机制。