Simultaneous Activation of Peroxydisulfate and Hydrogen Peroxide by Sulfidated Nanoscale Zero-Valent Iron for Efficient MTBE Degradation: Significant Role of Oxygen Vacancy,ACS ES&T Water

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Simultaneous Activation of Peroxydisulfate and Hydrogen Peroxide by Sulfidated Nanoscale Zero-Valent Iron for Efficient MTBE Degradation: Significant Role of Oxygen Vacancy
ACS ES&T Water ( IF 4.8 ) Pub Date : 2023-03-27 , DOI: 10.1021/acsestwater.3c00002
Jiaolong Qin _{1,

2} , Yan Wei ₁ , Wei Geng ₁ , Xiaojuan Yu ₁ , Baoxue Zhou ₁ , Mingce Long ₁

Affiliation

Nanoscale zero-valent iron (nZVI)-based advanced oxidation processes (AOPs) are limited by the rapidly formed surface layer of iron (oxyhydr) oxides. This restriction can be broken by the simultaneous activation of H₂O₂ and peroxydisulfate (PDS, S₂O₈^2–) over sulfidated nanoscale ZVI (S-nZVI), which displayed a synergistic effect to alleviate the drawbacks of the oxidants used alone. In this work, a biochar-supported S-nZVI (noted as S-nZVI@BC) was employed to simultaneously activate PDS and H₂O₂ for methyl tert-butyl ether (MTBE) degradation, and the rate constant for S-nZVI@BC/Bi-ox (Bi-ox, bi-oxidant at 1:1 molar ratio of PDS and H₂O₂) was 3.7-, 4.5-, and 12.8-fold higher than that of nZVI@BC/Bi-ox, S-nZVI@BC/PDS, and S-nZVI@BC/H₂O₂. According to electron paramagnetic resonance (EPR), X-ray photoelectric spectroscopy (XPS), and in-situ oxygen detection analyses, oxygen vacancies were generated over the shell of S-nZVI@BC during PDS activation, and the oxygen vacancy-contained surface layers promoted H₂O₂ adsorption and dissociation to produce surface-bound ^·OH (^·OH_ads), thus significantly improving H₂O₂ utilization efficiency and accelerating MTBE degradation. These findings provide promising S-nZVI-based AOPs by combining H₂O₂ and peroxydisulfate activation for environmental remediation and bring insights for the creation of oxygen vacancy-containing materials for peroxide activation.

中文翻译：

硫化纳米级零价铁同时激活过二硫酸盐和过氧化氢以高效降解 MTBE：氧空位的重要作用

基于纳米级零价铁 (nZVI) 的高级氧化工艺 (AOP) 受到快速形成的铁（羟基）氧化物表面层的限制。通过在硫化纳米级 ZVI (S-nZVI) 上同时激活 H ₂ O ₂和过二硫酸盐 (PDS, S ₂ O ₈^2– )可以打破这种限制，这显示出协同效应，可以减轻单独使用氧化剂的缺点. 在这项工作中，采用生物炭支持的 S-nZVI（记为 S-nZVI@BC）同时激活 PDS 和 H ₂ O ₂以降解甲基叔丁基醚 (MTBE)，以及 S-nZVI 的速率常数@BC/Bi-ox（Bi-ox，PDS 和 H ₂ O摩尔比为 1:1 的双氧化剂_{2 )比nZVI@BC/Bi-ox、S-nZVI@BC/PDS、S-nZVI@BC/H}₂ O ₂高3.7、4.5、12.8倍。根据电子顺磁共振 (EPR)、X 射线光电能谱 (XPS) 和原位氧检测分析，在 PDS 活化过程中，S-nZVI@BC 的壳层上产生了氧空位，并且包含氧空位的表面层促进H ₂ O ₂吸附和解离产生表面结合的^· OH（^· OH _ads），从而显着提高H ₂ O ₂利用效率和加速 MTBE 降解。_{这些发现通过将 H 2} O ₂和过二硫酸盐活化结合用于环境修复，提供了有前途的基于 S-nZVI 的 AOP ，并为创建用于过氧化物活化的含氧空位材料提供了见解。

更新日期：2023-03-27

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