State Key Laboratory of Petroleum Pollution Control, Beijing 102206, China; School of Environment & Natural Resource, Renmin University of China, Beijing 100872, China E-mail:
School of Environment & Natural Resource, Renmin University of China, Beijing 100872, China E-mail:
Water Sci Technol. 2019 May;79(9):1675-1684. doi: 10.2166/wst.2019.166.
FeNiCeO was firstly prepared by ultrasonic impregnation method and used to remove diclofenac in a Fenton-like system. The catalytic activity was improved successfully by doping Ni into FeCeO. The diclofenac removal efficiency reached 97.9% after 30 min reaction. The surface morphology and properties of FeNiCeO were characterized by Brunauer-Emmett-Teller (BET), scanning electron microscopy (SEM), X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), Raman and X-ray photoelectron spectroscopy (XPS) analyses. FeNiCeO in this paper had larger specific surface area than those prepared by other methods, which was attributed to the cavitation effect and hot-spot effect during the ultrasonic synthesis process. Low crystallinity of FeO and NiO showed by characterization could lead to high interaction of Fe and Ni ions with support of CeO. They substituted Ce in CeO, caused lattice contraction and formed more oxygen vacancies, which favoured the catalytic reaction. Meanwhile, Fe and Ce ions both had redox cycles of Fe/Fe and Ce/Ce, which facilitated the electron transfer in the reaction. The synergistic effect among Fe, Ni and Ce might lead to better catalytic performance of FeNiCeO than any binary metal oxides constituted from the above three elements. Finally, the potential mechanism of diclofenac removal in FeNiCeO-HO system is proposed.
采用超声浸渍法制备了 FeNiCeO，并将其用于芬顿-like 体系中去除双氯芬酸。通过向 FeCeO 中掺杂 Ni，成功提高了其催化活性。在 30 min 的反应后，双氯芬酸的去除效率达到了 97.9%。采用比表面积测试（BET）、扫描电子显微镜（SEM）、X 射线衍射（XRD）、高分辨率透射电子显微镜（HRTEM）、拉曼（Raman）和 X 射线光电子能谱（XPS）分析对 FeNiCeO 的表面形貌和性质进行了表征。与其他方法制备的样品相比，本文制备的 FeNiCeO 具有更大的比表面积，这归因于超声合成过程中的空化效应和热点效应。通过表征发现 FeO 和 NiO 结晶度较低，这可能导致 Fe 和 Ni 离子与 CeO 载体之间具有较高的相互作用。它们取代了 CeO 中的 Ce，引起晶格收缩并形成更多的氧空位，有利于催化反应的进行。同时，Fe 和 Ce 离子都具有 Fe/Fe 和 Ce/Ce 的氧化还原循环，这促进了反应中的电子转移。Fe、Ni 和 Ce 之间的协同效应可能导致 FeNiCeO 具有比由上述三种元素组成的任何二元金属氧化物更好的催化性能。最后，提出了在 FeNiCeO-HO 体系中去除双氯芬酸的潜在机制。
