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普鲁士蓝类似物衍生的零价铁通过活性氧和高价铁氧配合物有效激活过一硫酸盐以降解苯酚。

Prussian blue analogues-derived zero valent iron to efficiently activate peroxymonosulfate for phenol degradation triggered via reactive oxygen species and high-valent iron-oxo complexes.

作者信息

Wei Tong, Zhu Xin-Sheng, Wang Qi-Xue, Xu Ke-Ke, Tang Fu-Kai, Zhang Ming-Zhu, Lv Shi-Wen, Ge Feng

机构信息

Nanjing Institute of Environmental Science, MEE, Nanjing, 210042, China; Nanjing Guohuan Institute of Environmental Research CO. LTD, Nanjing, 210042, China.

Nanjing Institute of Environmental Science, MEE, Nanjing, 210042, China.

出版信息

Environ Res. 2023 Nov 15;237(Pt 1):116962. doi: 10.1016/j.envres.2023.116962. Epub 2023 Aug 22.

Abstract

It is of great significance to develop the effective technique to treat phenol-containing wastewater. Herein, Fe-based prussian blue analogues-derived zero valent iron (ZVI) was successfully synthesized by one-step calcination method. Owing to high specific surface area and rich active sites, ZVI-2 possessed excellent performance in charge transfer. Notably, in comparison with conventional ZVI and Fe, ZVI-2 can effectively activate peroxymonosulfate (PMS) for achieving rapid degradation of phenol, and the highest removal efficiency of phenol reached 94.9% within 24 min. More importantly, developed ZVI-2/PMS oxidation system with good stability displayed strong anti-interference capability. Interestingly, Fe loaded on the surface of ZVI-2 can efficiently break the O-O bond of PMS to generate reactive oxygen species (i.e., SO, OH, O and O). As main adsorption sites of PMS, the existence of oxygen vacancy promote the formation of high-valent transition metal complexes (namely ZVI-2≡Fe=O). Under the combined action of reactive oxygen species and ZVI-2≡Fe=O, phenol can be eventually degraded into CO and HO. The possible degradation pathways of phenol were also investigated. Furthermore, proposed ZVI-2/PMS oxidation system displayed great potential for application in the field of wastewater treatment. All in all, current work provided a valuable reference for design and application of Fe-based catalysts in PS-AOPs.

摘要

开发有效的含酚废水处理技术具有重要意义。在此,通过一步煅烧法成功合成了铁基普鲁士蓝类似物衍生的零价铁(ZVI)。由于具有高比表面积和丰富的活性位点,ZVI-2在电荷转移方面表现出优异的性能。值得注意的是,与传统的ZVI和Fe相比,ZVI-2能够有效活化过一硫酸盐(PMS)以实现苯酚的快速降解,在24分钟内苯酚的最高去除效率达到94.9%。更重要的是,所开发的具有良好稳定性的ZVI-2/PMS氧化体系表现出强大的抗干扰能力。有趣的是,负载在ZVI-2表面的Fe能够有效断裂PMS的O-O键以产生活性氧物种(即SO、OH、O和O)。作为PMS的主要吸附位点,氧空位的存在促进了高价态过渡金属配合物(即ZVI-2≡Fe=O)的形成。在活性氧物种和ZVI-2≡Fe=O的共同作用下,苯酚最终可降解为CO和HO。还研究了苯酚可能的降解途径。此外,所提出的ZVI-2/PMS氧化体系在废水处理领域显示出巨大的应用潜力。总而言之,当前的工作为铁基催化剂在PS-AOPs中的设计和应用提供了有价值的参考。

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