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Hydrophilic mesoporous carbon as iron(III)/(II) electron shuttle for visible light enhanced Fenton-like degradation of organic pollutants
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2018-03-06 , DOI: 10.1016/j.apcatb.2018.03.016
Xufang Qian , Meng Ren , Mengyuan Fang , Miao Kan , Dongting Yue , Zhenfeng Bian , Hexing Li , Jinping Jia , Yixin Zhao

A Fenton-like catalyst comprising of hydrophilic mesoporous carbon (HMC) and ferric ions was found very efficiently in degradation organic pollutants under visible light irradiation in the presence of H2O2. HMC with graphene domains and plenty of oxygen containing groups such as carboxyl groups can cooperate with ferric ions to form a visible light active Fe(III)-HMC configuration. Fe(III)-HMC showed obviously enhanced phenol degradation and mineralization efficiencies than that in dark condition. Acidic condition (pH = 3) is not only more superior in phenol degradation but also in iron leaching in comparison with the case at basic conditions (pH = 4.5–7.0) for Fe(III)-HMC. Total organic carbon (TOC) removal efficiency of five typical organic pollutants show that visible light active Fe(III)-HMC catalyst is more efficient than homogeneous Fenton reagents FeSO4/H2O2 excluding the temperature effect. Electron spin resonance (ESR) and electrochemical measurements reveal that the presence of active phenoxyl radicals and ligand to metal charge transfer (LMCT) facilitates the cycling of Fe(III)/Fe(II) and inhibit the side reaction via Haber-Weiss reaction. ·OH radicals rather than O2− and OOH were proved as the predominantly active oxidant. The proposed Fe(III)-HMC configuration activated by visible light opens up a new strategy for carbon based materials and iron species in Fenton-like chemistry.



中文翻译:

亲水介孔碳作为铁(III)/(II)电子梭,用于可见光,可增强芬顿样降解有机污染物的能力

发现在H 2 O 2存在下,在可见光照射下,由亲水介孔碳(HMC)和三价铁离子组成的Fenton型催化剂非常有效地降解了有机污染物。。具有石墨烯结构域和大量含氧基团(例如羧基)的HMC可以与铁离子配合形成可见光活性Fe(III)-HMC构型。Fe(III)-HMC比黑暗条件下的苯酚降解和矿化效率明显提高。与碱性条件(pH = 4.5-7.0)下的Fe(III)-HMC相比,酸性条件(pH = 3)不仅在苯酚降解方面更优越,而且在铁浸出方面也更优越。五个典型有机污染物的总有机碳(TOC)去除效率表明,可见光活性Fe(III)-HMC催化剂比均相Fenton试剂FeSO 4 / H 2 O 2更有效排除温度影响。电子自旋共振(ESR)和电化学测量表明,活性苯氧基自由基和配体向金属的电荷转移(LMCT)的存在促进了Fe(III)/ Fe(II)的循环并通过Haber-Weiss反应抑制了副反应。·OH自由基而不是O 2−OOH被证明是主要的活性氧化剂。拟议的Fe(III)-HMC构型由可见光激活,为类芬顿化学中的碳基材料和铁物种开辟了新的策略。

更新日期:2018-03-06
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