Wei Chenmo, Zhang Jing, Zhang Yongli, Zhang Gucheng, Zhou Peng, Li Wenshu, Liang Juan, Liu Ya, Zhang Wei
College of Architecture and Environment, Sichuan University, Chengdu 610065, China E-mail:
Water Sci Technol. 2017 Sep;76(5-6):1436-1446. doi: 10.2166/wst.2017.316.
Sulfate radical-based advanced oxidation processes have had considerable attention due to the highly oxidizing function of sulfate radicals (SO·) resulting in acceleration of organic pollutants degradation in aqueous environments. A Co-Ni mixed oxide nanocatalyst, which was prepared by the sol-gel method, was employed to activate peroxymonosulfate (PMS, HSO) to produce SO· with Acid Orange 7 (AO7) selected as a radical probe. The catalyst was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR) and transmission electron microscopy (TEM). The characterization results indicated that the ingredient of the catalyst had been changed and the amount of surface hydroxyl increased significantly with the addition of Ni. Therefore, it proved that Co-NiOx catalyst was more effective than CoOx to activate PMS. Moreover, ultrasound (US) can increase the degradation rate of AO7 and US/Co-NiOx/PMS system. This study also focused on some synthesis parameters and the system reached the maximum efficiency under the condition when [PMS] = 0.4 mM, [catalyst] = 0.28 g/L, Pus = 200 W. The AO7 removal in these systems follows first order kinetics. Last but not least, quenching studies was conducted which indicated that the amount of hydroxyl radicals (·OH) increases with the increase of initial pH and SO· was the primary reactive oxidant for AO7 degradation.
基于硫酸根自由基的高级氧化过程因其硫酸根自由基(SO·)的高氧化功能而备受关注,该功能可加速水环境中有机污染物的降解。采用溶胶-凝胶法制备的Co-Ni混合氧化物纳米催化剂用于活化过一硫酸盐(PMS,HSO)以产生SO·,选择酸性橙7(AO7)作为自由基探针。通过X射线衍射(XRD)、X射线光电子能谱(XPS)、傅里叶变换红外光谱(FT-IR)和透射电子显微镜(TEM)对催化剂进行了表征。表征结果表明,添加Ni后催化剂成分发生了变化,表面羟基数量显著增加。因此,证明Co-NiOx催化剂比CoOx更有效地活化PMS。此外,超声(US)可提高AO7的降解速率以及US/Co-NiOx/PMS体系的降解速率。本研究还关注了一些合成参数,当[PMS]=0.4 mM、[催化剂]=0.28 g/L、Pus=200 W时,该体系达到最大效率。这些体系中AO7的去除遵循一级动力学。最后但同样重要的是,进行了猝灭研究,结果表明羟基自由基(·OH)的数量随初始pH值的增加而增加,且SO·是AO7降解的主要活性氧化剂。