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Catalytic activity of different iron oxides: Insight from pollutant degradation and hydroxyl radical formation in heterogeneous Fenton-like systems
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2018-07-05 , DOI: 10.1016/j.cej.2018.07.035
Ling Zhao , Zhi-Rong Lin , Xiao-hong Ma , Yuan-Hua Dong

The catalytic performance of iron oxides in 2,4,4′-trichlobiphenyl (PCB28) degradation following an order of goethite > magnetite > hydrated iron(III) oxide > hematite was observed in four iron oxides catalyzed Fenton-like reactions, which was not consistent with the stoichiometric efficiency of OH generation. This result indicates that OH was not the sole active species responsible for PCB28 degradation in four iron oxides catalyzed Fenton-like systems. The reductive degradation of hexachloroethane (HCE) was 76.8%, 58.7%, 46.1% and 37.6% for magnetite, goethite, hematite and hydrated iron(III) oxide, respectively, further suggesting that both oxidative species (OH) and reductive species (HO2) simultaneously contributed on PCB28 degradation. The addition of tert-butyl alcohol (OH scavenger) decreased the amount of 7-hydroxycoumarin (7-HC, OH indicator) by 42%, 77%, 97%, and 97% for magnetite, goethite, hematite, and hydrated iron(III) oxide, respectively. Meanwhile, the addition of p-benzoquinone (HO2 scavenger) only reduced the amount of 7-HC by 77%, 27%, and 33.5% for magnetite, hematite, and hydrated iron(III) oxide, respectively; but increased the amount of 7-HC by 126.7% in the goethite/H2O2 system. This result indicates that the mechanism of OH generation from H2O2 catalyzed by four iron oxides was different. For goethite, the surface lattice iron was primarily responsible for activating H2O2 to form reactive species (OH and HO2) and thereby degrade pollutants on the oxide surface. For magnetite, both the surface lattice iron and the dissolved Fe in solution played an equally important role in catalyzing H2O2 decomposition to form and propagate reactive species for pollutant degradation. For hematite and hydrated iron(III) oxide, the solution phase chain reaction effectively propagated by dissolved Fe should be the primary catalytic mechanism although the chain reaction was initiated by the surface processes.



中文翻译:

不同铁氧化物的催化活性:异质类芬顿体系中污染物降解和羟基自由基形成的见解

在四种铁氧化物催化的Fenton样反应中观察到氧化铁在针铁矿>磁铁矿>水合氧化铁(III)>赤铁矿的顺序中对2,4,4'-三氟苯基(PCB28)降解的催化性能。与OH生成的化学计量效率一致。该结果表明,在四种铁氧化物催化的Fenton样体系中,OH并不是引起PCB28降解的唯一活性物质。磁铁矿,针铁矿,赤铁矿和水合氧化铁(III)的六氯乙烷(HCE)的还原降解分别为76.8%,58.7%,46.1%和37.6%,这进一步表明了氧化性(OH)和还原性(HO)2)同时导致PCB28退化。的加法丁醇(OH清除剂)对磁铁矿,针铁矿,赤铁矿和水合氧化铁(III)的7-羟基香豆素(7-HC,OH指示剂)的含量降低了42%,77%,97%和97% , 分别。同时,对-醌(HO 2清除剂)的添加仅使磁铁矿,赤铁矿和水合氧化铁(III)的7-HC含量分别减少了77%,27%和33.5%。但在针铁矿/ H 2 O 2体系中将7-HC的含量提高了126.7%。该结果表明由H 2 O 2生成OH的机理四种氧化铁的催化作用是不同的。对于针铁矿,表面晶格铁主要负责活化H 2 O 2形成反应性物质(OH和HO 2),从而降解氧化物表面上的污染物。对于磁铁矿,表面晶格铁和溶液中溶解的铁在催化H 2 O 2分解以形成和传播用于污染物降解的反应性物种方面起着同等重要的作用。对于赤铁矿和水合氧化铁(III),尽管链反应是由表面过程引发的,但固溶有效传播的固溶链反应应该是主要的催化机理。

更新日期:2018-07-05
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