Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-01-20 , DOI: 10.1016/j.apcatb.2020.118665 Jun Zhang , Gong Zhang , Qinghua Ji , Huachun Lan , Jiuhui Qu , Huijuan Liu
Achieving efficient production and activation of H2O2 is a promising strategy to enhance the efficiency of heterogeneous Fenton reactions. For this purpose, an ideal heterogeneous Fenton platform was constructed though chemical embedding of carbon nanodots (CDots) onto the surface of iron oxychloride (FeOCl/CDots). Experimental results and theoretical calculations confirmed that CDots acted as the reactive sites for highly effective separation of photogenerated electrons and holes in the FeOCl substrate, whereby the O2 molecules in solution could be synchronously reduced to H2O2 via a two-electron pathway (O2 → •O2H → H2O2) on the CDots. Under visible light irradiation, the concentration of H2O2 accumulated to ∼337.2 μmol L−1 in the FeOCl/CDots system, which was almost ∼14 times higher than that using FeOCl alone. Moreover, the FeOCl substrate with abundant Fe2+ could directly capture and activate the H2O2 to produce abundant hydroxyl radical (•OH), thereby effectively avoiding the H2O2 mass transfer limitation encountered in traditional heterogeneous Fenton reactions. In experiments with a typical organic contaminant (p-chlorophenol), the oxidation rate and mineralization efficiency in this Fenton system were ∼4 and ∼6 times higher than that achieved using FeOCl alone.
中文翻译:
碳纳米点修饰的FeOCl用于光辅助Fenton反应,具有协同原位H 2 O 2的产生和活化
实现H 2 O 2的有效产生和活化是提高异质Fenton反应效率的有前途的策略。为此,通过将碳纳米点(CDots)化学嵌入氧氯化铁(FeOCl / CDots)的表面,构建了理想的异质Fenton平台。实验结果和理论计算证实,CDots可以作为高效分离FeOCl衬底中光生电子和空穴的反应位点,从而溶液中的O 2分子可以通过双电子途径同步还原为H 2 O 2( O 2 →•O 2 H→H 2 O2)在CDots上。在可见光照射下,FeOCl / CDots系统中的H 2 O 2浓度累积至约337.2μmolL -1,几乎是单独使用FeOCl时的约14倍。而且,具有丰富的Fe 2+的FeOCl底物可以直接捕获并激活H 2 O 2以产生丰富的羟基自由基(•OH),从而有效地避免了H 2 O 2的产生。传统的非均质Fenton反应遇到传质限制。在典型的有机污染物(对氯苯酚)的实验中,该Fenton系统的氧化速率和矿化效率分别比单独使用FeOCl时高约4倍和约6倍。