Laboratory of Environmental Technology, INET, Tsinghua University, Beijing, People's Republic of China.
Environ Sci Technol. 2012 Sep 18;46(18):10145-53. doi: 10.1021/es300303f. Epub 2012 Sep 5.
Magnetic nanoscaled Fe(3)O(4)/CeO(2) composite was prepared by the impregnation method and characterized as a heterogeneous Fenton-like catalyst for 4-chlorophenol (4-CP) degradation. The catalytic activity was evaluated in view of the effects of various processes, pH value, catalyst addition, hydrogen peroxide (H(2)O(2)) concentration, and temperature, and the pseudo-first-order kinetic constant of 0.11 min(-1) was obtained for 4-CP degradation at 30 °C and pH 3.0 with 30 mM H(2)O(2), 2.0 g L(-1) Fe(3)O(4)/CeO(2), and 0.78 mM 4-CP. The high utilization efficiency of H(2)O(2), calculated as 79.2%, showed a promising application of the catalyst in the oxidative degradation of organic pollutants. The reusability of Fe(3)O(4)/CeO(2) composite was also investigated after six successive runs. On the basis of the results of metal leaching, the effects of radical scavengers, intermediates determination, and X-ray photoelectron spectroscopic (XPS) analysis, the dissolution of Fe(3)O(4) facilitated by CeO(2) played a significant role, and 4-CP was decomposed mainly by the attack of hydroxyl radicals (•OH), including surface-bound •OH(ads) generated by the reaction of Fe(2+) and Ce(3+) species with H(2)O(2) on the catalyst surface, and •OH(free) in the bulk solution mainly attributed to the leaching of Fe.
磁性纳米 Fe(3)O(4)/CeO(2) 复合材料通过浸渍法制备,并被用作类芬顿非均相催化剂用于降解 4-氯苯酚(4-CP)。从各种工艺条件、pH 值、催化剂添加量、过氧化氢(H(2)O(2))浓度和温度的影响方面评估了其催化活性,在 30°C 和 pH 值 3.0 下,用 30mM H(2)O(2)、2.0gL(-1)Fe(3)O(4)/CeO(2)和 0.78mM 4-CP 处理时,4-CP 降解的表观一级动力学常数为 0.11min(-1)。H(2)O(2)的高利用率(79.2%)表明该催化剂在有机污染物的氧化降解方面具有广阔的应用前景。在六次连续运行后,还研究了 Fe(3)O(4)/CeO(2) 复合材料的可重复使用性。根据金属浸出的结果、自由基清除剂的影响、中间产物的确定和 X 射线光电子能谱(XPS)分析,CeO(2) 促进的 Fe(3)O(4)溶解起着重要作用,4-CP 主要通过羟基自由基(•OH)的攻击而分解,包括由催化剂表面上 Fe(2+)和 Ce(3+)物种与 H(2)O(2)反应生成的表面结合的•OH(ads),以及主要归因于 Fe 浸出的体相中的•OH(free)。