Fe doped CeO2 nanosheets as Fenton-like heterogeneous catalysts for degradation of salicylic acid
Fe doped CeO2 nanosheets as Fenton-like heterogeneous catalysts for degradation of salicylic acid
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DOI：
10.1016/j.cej.2017.08.065
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发表时间：
2018-02
影响因子：
15.1
通讯作者：
Wei Wang;Qin Zhu;F. Qin;Qiguang Dai;Xingyi Wang
中科院分区：
文献类型：
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作者：
Wei Wang;Qin Zhu;F. Qin;Qiguang Dai;Xingyi Wang
采用溶剂热法（ST）合成了不同Fe/Ce比例的Fe掺杂CeO2纳米片，并通过H2O2存在下水杨酸（SA）的降解（类芬顿氧化）来评价其催化性能。通过SEM、TEM、XRD、EPR、拉曼、H2-TPR和XPS对Fe-CeO2混合氧化物进行表征，结果表明，由于SA和H2O2在表面Ce3+上的复合吸附，2%Fe掺杂CeO2纳米片（2Fe-CeO2）在最佳反应条件下表现出最大浓度的表面氧空位和最高的催化活性。 DMPO自旋捕获EPR研究和中间产物的LC-MS分析表明超氧化物物种（O2自由基点−/HOO自由基点）在氧化降解过程中起着至关重要的作用，同时提出了SA降解的可能途径。未完全降解的低分子量有机酸（LMWOA）在活性位点上的强烈吸附降低了2Fe-CeO2催化剂的可重复使用性，然而，通过在空气气氛中简单的煅烧处理可以恢复催化活性。
Fe doped CeO2nanosheets with various Fe/Ce ratios were synthesized by solvothermal method (ST) and catalytic performances were evaluated by the degradation of salicylic acid (SA) in the presence of H2O2(Fenton-like oxidation). The Fe-CeO2mixed oxides were characterized by SEM, TEM, XRD, EPR, Raman, H2-TPR and XPS, which indicated that 2% Fe doped CeO2nanosheets (2Fe-CeO2) showed the largest concentration of surface oxygen vacancies and the highest catalytic activity under the optimum reaction conditions due to the complex adsorption of SA and H2O2on the surface Ce3+. DMPO spin trapping EPR studies and analysis of intermediate products by LC-MS indicated that superoxide species (O2radical dot−/HOOradical dot) played a crucial role in the oxidation degradation process, meanwhile, the probable pathway of SA degradation was proposed. The strong adsorption of not-fully degraded low molecular weight organic acids (LMWOAs) on the active sites decreased the reusability of 2Fe-CeO2catalyst, however, the catalytic activities could be recovered by a simple calcination treatment in air atmosphere.