School of Chemistry & Environment, South China Normal University, Guangdong Provincial Engineering Technology Research Center for Drinking Water Safety, Key Laboratory of Theoretical Chemistry of Environment, Ministry of Education, Guangzhou 510006, China.
School of Chemistry & Environment, South China Normal University, Guangdong Provincial Engineering Technology Research Center for Drinking Water Safety, Key Laboratory of Theoretical Chemistry of Environment, Ministry of Education, Guangzhou 510006, China.
Chemosphere. 2018 Sep;206:615-621. doi: 10.1016/j.chemosphere.2018.05.066. Epub 2018 May 12.
Fe-MCM-48 catalyst with a three-dimensional cubic pore structure was directly synthesized via a hydrothermal method, and the mineralization efficiency of diclofenac (DCF) in the catalytic ozonation process (Fe-MCM-48/O) was assessed. X-ray diffraction (XRD), N adsorption desorption, transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) characterizations revealed that Fe existed in the framework of MCM-48, and Fe-MCM-48 possessed a large surface area and a highly ordered cubic mesoporous structure, which could accelerate reactants and products diffusion. Regarding mineralization efficiency, the addition of Fe-MCM-48 significantly improved total organic carbon (TOC) removal, and approximately 49.9% TOC were removed through the Fe-MCM-48/O process at 60 min, which was 2.0 times higher than that in single ozonation. Due to this catalyst's superior structure, Fe-MCM-48 showed the better catalytic activity compared with Fe-MCM-41 and Fe loaded MCM-48 (Fe/MCM-48, Fe existed on the surface of MCM-48). DCF removal in the Fe-MCM-48/O process was primarily based on ozone direct oxidation. The improvement of mineralization efficiency was attributed to the function of generated hydroxyl radicals (•OH), which indicated that the presence of Fe-MCM-48 accelerated ozone decomposition. Moreover, the negatively charged surface of Fe-MCM-48 and the proper pH value of the DCF solution played an essential role in OH generation.
采用水热法直接合成具有三维立方孔结构的 Fe-MCM-48 催化剂，并评估了其在催化臭氧化过程（Fe-MCM-48/O）中对双氯芬酸（DCF）的矿化效率。X 射线衍射（XRD）、N 吸附脱附、透射电子显微镜（TEM）和 X 射线光电子能谱（XPS）表征表明，Fe 存在于 MCM-48 的骨架中，并且 Fe-MCM-48 具有较大的比表面积和高度有序的立方介孔结构，这可以加速反应物和产物的扩散。关于矿化效率，添加 Fe-MCM-48 显著提高了总有机碳（TOC）的去除率，在 60 分钟的 Fe-MCM-48/O 过程中，TOC 的去除率约为 49.9%，比单独臭氧化高 2.0 倍。由于该催化剂具有优越的结构，Fe-MCM-48 表现出比 Fe-MCM-41 和负载 Fe 的 MCM-48（Fe 存在于 MCM-48 的表面）更好的催化活性。Fe-MCM-48/O 过程中 DCF 的去除主要基于臭氧的直接氧化。矿化效率的提高归因于生成的羟基自由基（•OH）的作用，这表明 Fe-MCM-48 的存在加速了臭氧的分解。此外，Fe-MCM-48 的带负电荷表面和 DCF 溶液的适当 pH 值在 OH 生成中起着重要作用。
