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用于增强高级氧化过程中 Fe(III)/Fe(II)氧化还原循环的赤铁矿/二硫化硒杂化催化剂。

Hematite/selenium disulfide hybrid catalyst for enhanced Fe(III)/Fe(II) redox cycling in advanced oxidation processes.

机构信息

School of Environment and Energy, South China University of Technology, Guangzhou, Guangdong 510006, China; Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, MO 63130, USA.

School of Environment and Energy, South China University of Technology, Guangzhou, Guangdong 510006, China.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt A):127376. doi: 10.1016/j.jhazmat.2021.127376. Epub 2021 Sep 29.

Abstract

Regeneration of Fe(II) is a key issue for heterogeneous advanced oxidation processes (AOPs) using iron-based catalysts. Herein, a hybrid catalyst was developed from α-FeO and SeS to enhance the Fe(III)/Fe(II) redox cycling in both hydrogen peroxide (HO) system and persulfate (PS) system. The regeneration of Fe(II) was evidenced by the increased Fe(II)/Fe(III) ratio in the used catalyst (205.8% in the HO system or 125.4% in the PS system), compared to 68.4% in the fresh hybrid catalyst Fe/Se-3. Methyl orange was used as a model pollutant to evaluate the degradation performance of the hybrid catalyst. Owing to the promotion of Fe(II) regeneration, Fe/Se-3 achieved a pollutant removal efficiency of 100.0% in 12 min in both systems, significantly higher than that with pure α-FeO (33.9 ± 3.6% in the HO system or 30.7 ± 2.8% in the PS system). The dominant active species were identified as hydroxyl radicals in the HO system and sulfate radicals in the PS system. In the proposed mechanism, soluble and surface-bound Fe species are provided by α-FeO to activate HO or PS to radicals, and SeS participates in the reactions via Se(IV) reducing Fe(III) to Fe(II) and S atoms being released through protonation to expose more active Se sites.

摘要

再生亚铁是使用铁基催化剂的多相高级氧化过程(AOPs)的关键问题。在此,开发了一种由α-FeO 和 SeS 组成的混合催化剂,以增强过氧化氢(HO)系统和过硫酸盐(PS)系统中 Fe(III)/Fe(II) 的氧化还原循环。通过增加用过的催化剂中的 Fe(II)/Fe(III) 比值(HO 系统中为 205.8%,PS 系统中为 125.4%),证明了 Fe(II) 的再生,而新鲜的混合催化剂 Fe/Se-3 的比值为 68.4%。使用甲基橙作为模型污染物来评估混合催化剂的降解性能。由于促进了 Fe(II)的再生,Fe/Se-3 在两种系统中 12 分钟内实现了 100.0%的污染物去除效率,明显高于纯α-FeO 的去除效率(HO 系统中为 33.9±3.6%,PS 系统中为 30.7±2.8%)。在提出的机制中,α-FeO 提供了可溶性和表面结合的铁物种,以将 HO 或 PS 激活为自由基,而 SeS 通过 Se(IV) 将 Fe(III)还原为 Fe(II)并通过质子化释放 S 原子来参与反应,从而暴露更多的活性 Se 位。

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