A hypervalent metal MOF catalyst as an avenue to go beyond heterogeneous Fenton-like processes for organic contaminant removal in water†

IF 4.7 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Lucas Santos-Juanes, Noelia Rodriguez-Sanchez, Salvador R. G. Balestra, Nuria O. Núñez, Antonio Arques, A. Rabdel Ruiz-Salvador and Menta Ballesteros
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Abstract

Metal–organic frameworks (MOFs) have recently been proposed as a plausible solution to the pressing issue of water scarcity and as a means of remediating contaminated water bodies. In light-assisted water treatment, they have so far only been exploited via the hydroxyl radical route, through Fenton-like processes. A new avenue is introduced here by the biomimetic conceptual design of MOF bearing hypervalent metal atoms for photocatalytic water treatment. We report a zeolitic imidazole framework (ZIF) material doped with iron (Fe-ZIF-7-III; UPO-4) synthesized via a novel mild treatment to stabilize photoactive hypervalent ferryl ions for the first time in a MOF for water treatment. The successful synthesis of the 2D material and the adequate incorporation of iron into the structure were demonstrated using X-ray diffraction (XRD), Fourier-transform infrared (FTIR) spectroscopy, and scanning electron microscopy (SEM). A simulation study analyzed the structure and stability of the Fe-ZIF-7-III material as well as the involvement of ferryl ions in the photo-Fenton-type process. Furthermore, the calculated band gap of this material shows its viability for use in photocatalysis using sunlight. This was confirmed by evaluating the photodegradation of caffeine, a model pollutant in water, without the assistance of hydroxyl radicals as indicated by a scavenger test. The recyclability test revealed that Fe-ZIF-7-III could be used continuously with effective catalytic activity, thus opening the door to the field of studying hypervalent metal MOFs not yet explored in water treatment.

Abstract Image

高价金属MOF催化剂是一种超越非均相fenton类工艺去除水中有机污染物的途径
金属有机框架(MOFs)最近被认为是解决紧迫的水资源短缺问题和修复受污染水体的一种可行的方法。在光辅助水处理中,到目前为止,它们只通过羟基自由基途径,通过芬顿样过程被利用。本文介绍了含高价金属原子的MOF光催化水处理的仿生概念设计。我们报道了一种掺杂铁的沸石咪唑骨架(ZIF)材料(Fe-ZIF-7-III;在水处理MOF中首次合成了稳定光活性高价铁基离子的新型温和处理方法UPO-4。通过x射线衍射(XRD)、傅里叶变换红外光谱(FTIR)和扫描电子显微镜(SEM)验证了二维材料的成功合成和铁在结构中的充分结合。模拟研究分析了Fe-ZIF-7-III材料的结构和稳定性以及铁离子在光- fenton型过程中的参与。此外,计算出的这种材料的带隙显示了它在利用太阳光进行光催化方面的可行性。这是通过评估咖啡因的光降解,一种模式污染物在水中,没有羟基自由基的帮助,由清除剂试验表明。可回收性试验表明,Fe-ZIF-7-III可以连续使用并具有有效的催化活性,从而为水处理中尚未探索的高价金属mof研究领域打开了大门。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Materials Advances
Materials Advances MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
7.60
自引率
2.00%
发文量
665
审稿时长
5 weeks
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