Hydrophilic mesoporous carbon as iron(III)/(II) electron shuttle for visible light enhanced Fenton-like degradation of organic pollutants
Hydrophilic mesoporous carbon as iron(III)/(II) electron shuttle for visible light enhanced Fenton-like degradation of organic pollutants
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亲水介孔碳作为铁（III）/（II）电子穿梭，用于可见光增强有机污染物的类芬顿降解
DOI：
10.1016/j.apcatb.2018.03.016
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发表时间：
2018
期刊：
影响因子：
--
通讯作者：
Zhao YX
中科院分区：
文献类型：
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作者：
Qian Xufang;Ren Meng;Fang Mengyuan;Kan Miao;Yue Dongting;Jia Jinping;Zhao Yixin;Bian Zhenfeng;Li Hexing;Bian Zhenfeng;Li Hexing;Zhao YX
在可见光照射下，发现由亲水性介孔碳(HMC)和铁离子组成的类Fenton催化剂对有机污染物的降解非常有效。具有石墨烯结构域和大量含氧基团(如羧基)的HMC可以与铁离子形成可见光活性的Fe(III)-HMC构型。与黑暗条件下相比，Fe(III)-HMC对苯酚的降解和矿化效率有明显提高。与碱性条件(pH = 4.5~7.0)相比，酸性条件(pH = 3)不仅对苯酚的降解效果更好，而且对铁的浸出性能也更好。5种典型有机污染物对总有机碳(TOC)的去除效果表明，除去温度的影响，可见光活性Fe(III)-HMC催化剂比均相Fenton试剂FeSO4/H_2O_2具有更高的去除效率。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对金属电荷转移(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自由基而不是点O2−和点OOH自由基是主要的活性氧化剂。被可见光激活的Fe(III)-HMC构型为碳基材料和铁物种在类Fenton化学中开辟了一种新的策略。
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/H2O2excluding 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 radical dotO2−and radical dotOOH 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.