One-step fabrication of oxygen vacancy-enriched Fe@Ti/C composite for highly efficient degradation of organic pollutants through persulfate activation.

One-step fabrication of oxygen vacancy-enriched Fe@Ti/C composite for highly efficient degradation of organic pollutants through persulfate activation.
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一步制备富氧空位的 Fe@Ti/C 复合材料,通过过硫酸盐活化高效降解有机污染物。

DOI:
10.1016/j.jcis.2020.09.064
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发表时间:
2020-09
影响因子:
9.9
通讯作者:
Wang Hui
Wang Hui
中科院分区:
化学1区
文献类型:
--
作者:
Xie Ruzhen;Jiang Yanbin;Armutlulu Andac;Shen Ziye;Lai Bo;Wang Hui

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本文利用微波炉一步碳热还原钛铁矿的方法合成了高性价比、高活性中心的磁性碳负载Fe@Ti复合材料(Fe@Ti/Cs),并将其作为高效的过硫酸盐(PS)活化剂用于废水净化。Fe@Ti/Cs上Fe0/2+/3+、Ti3+/4+和氧空位的共存有利于电子向PS的转移,有利于活性氧(ROS)的产生。催化实验结果表明,钛铁矿/炭质量比为4:1制备的Fe@Ti/C-4催化剂对PS降解罗丹明B(RhB)表现出最好的催化活性。在含PS的体系中,仅用0.12g/L Fe@Ti/C-4即可在30min内去除94.01%的RhB(200g/L),明显优于相同条件下测试的钛铁矿+PPS(29.29%)和碳源+PPS(49.91%)系统。对反应前后的Fe@Ti/Cs的物化性能进行了详细的表征。进行了自由基清除实验和电子顺磁共振(EPR)分析,以更好地了解其内在机理。结果表明,在含PS的体系中,Fe@Ti/C-4中的氧空位促进了电子转移,参与了过渡金属氧化还原循环,生成了ROS,从而高效地将RhB降解成小分子,最终实现了矿化。这项工作为设计高效、稳定、寿命长的天然矿源PS活化剂提供了新的视角。
In this work, cost-effective, magnetic carbon-supported Fe@Ti composite (Fe@Ti/Cs) with abundant active sites was synthesized by one-step carbothermal reduction of ilmenite with the assistance of microwave oven and utilized as a highly efficient persulfate (PS) activator for the wastewater purification. The coexistence of Fe0/2+/3+, Ti3+/4+and oxygen vacancies on Fe@Ti/Cs was found to favor for the electron transfer to PS, which facilitate the generation of reactive oxygen species (ROS). Catalytic experiment results showed that the Fe@Ti/C-4 produced from ilmenite/carbon with a mass ratio of 4:1 exhibited the best catalytic activation performance towards PS for the degradation of Rhodamine B (RhB). Usage of merely 0.12 g/L Fe@Ti/C-4 enabled the removal of 94.01% RhB (200 mg/L) within 30 min in the PS containing system, significantly outperforming ilmenite + PS (29.29%) and carbon + PS (49.91%) systems tested under the same conditions. The physico-chemical properties of the produced Fe@Ti/Cs before and after the reaction were carefully characterized. Radical scavenging experiments and electron paramagnetic resonance (EPR) analysis were carried out to better understand the underlying mechanism. The results indicate that oxygen vacancies in Fe@Ti/C-4 promoted the electron transfer and participated in the transition metal redox cycle to generate ROS in the PS-containing system, which was highly efficient for degrading RhB into small molecules and finally enabling mineralization. This work offers a new perspective for designing highly efficient and stable PS activators with long life derived from natural ore for environmental remediation.
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