Catalytic oxidation of 1,2-dichlorobenzene over Ca-doped FeOx hollow microspheres
Catalytic oxidation of 1,2-dichlorobenzene over Ca-doped FeOx hollow microspheres
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DOI：
10.1016/j.apcatb.2013.10.003
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发表时间：
2014-04
影响因子：
22.1
通讯作者：
Xiaodong Ma;Xi Feng;Jie Guo;H. Cao;Xueyue Suo;Hongwen Sun;Meihua Zheng
中科院分区：
文献类型：
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作者：
Xiaodong Ma;Xi Feng;Jie Guo;H. Cao;Xueyue Suo;Hongwen Sun;Meihua Zheng
以碳微球为模板，成功制备了新型钙掺杂氧化铁空心微球。用火焰原子吸收光谱、X射线衍射仪、氮气吸附/脱附、扫描电子显微镜、透射电子显微镜、H2-TPR和XPS对催化剂进行了表征。通过1，2-二氯苯(o-DCB)的催化氧化反应评价了样品的催化活性。结果表明，中空微球中Ca/(Ca++)和Fe的摩尔比及其形貌对其催化性能有显著影响。低温催化活性按FeCa10、FeCa20、Fe2O3、FeCa5的顺序递减，与它们的还原顺序一致。优化后的FeCa10催化剂不仅具有良好的催化活性、耐水性和稳定性，而且具有较低的表观活化能(21.6kJ/mol)。原位FTIR测试表明，醋酸盐和甲酸盐物种是部分氧化产物，可以随后被氧化成二氧化碳。结果表明，FeCa10催化剂具有良好的催化性能，主要是由于其微晶尺寸小、表面活性氧浓度高、低温还原性能好以及CaO和Fe3O4之间的协同作用等因素共同作用的结果。我们有理由相信，这种钙掺杂的氧化铁空心微球是一种很有前途的氯化挥发性有机污染物消除催化剂。
Novel Ca-doped FeOxhollow microspheres were successfully prepared using carbon microspheres as templates. The as-prepared catalysts were characterized by FAAS, XRD, N2adsorption/desorption, SEM, TEM, H2-TPR and XPS. The catalytic activities of the samples were evaluated by catalytic oxidation of 1,2-dichlorobenzene (o-DCB). The results showed that the molar ratios of Ca/(Ca + Fe) in the hollow microspheres and their morphologies significantly affected their catalytic performances. The low-temperature catalytic activity decreased in the order of FeCa10 > FeCa20 > Fe2O3> FeCa5, in well agreement with the sequence of their reducibility. The optimal FeCa10 catalyst exhibited not only excellent catalytic activity, water-resistant performance and stability but also lower apparent activation energy (21.6 kJ/mol). In situ FTIR measurements revealed the acetate and formate species were the partial oxidation products, which could be subsequently oxidized to form CO2. It is concluded that the excellent catalytic performance of FeCa10 catalyst might be attributed to the combined effects of several factors such as small crystallite size, high surface active oxygen concentration, good low-temperature reducibility and the synergic effect between CaO and Fe3O4. It is reasonable for us to believe that such Ca-doped FeOxhollow microspheres are promising catalysts for the elimination of chlorinated volatile organic pollutants.