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扩大类芬顿反应降解污染物的pH范围:酸性微环境的影响。

Expanding the pH range of Fenton-like reactions for pollutant degradation: The impact of acidic microenvironments.

作者信息

Xu Shi-Lin, Wang Wei, Song Yi, Tang Rui, Hu Zhen-Hu, Zhou Xiao, Yu Han-Qing

机构信息

CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei 230026, China.

Anhui Provincial Engineering Laboratory for Rural Water Environment and Resources, School of Civil Engineering, Hefei University of Technology, Hefei 230009, China.

出版信息

Water Res. 2025 Feb 15;270:122851. doi: 10.1016/j.watres.2024.122851. Epub 2024 Nov 24.

DOI:10.1016/j.watres.2024.122851
PMID:39612819
Abstract

Heterogeneous Fenton reactions offer the opportunities to overcome iron sludge accumulation and limited recyclability of existing homogeneous Fenton process, but the sharp attenuation in their reactivity at near-neutral and even higher pH conditions, still remains a formidable challenge. In this work, we report a versatile and robust approach to create a local acidic microenvironment on BiOI with graphene oxide bonding, enabling the heterogeneous Fenton (BiOI@rGO/HO) system to sustainably degrade organic pollutants over a wide pH range (3.0-10.0). Notably, BiOI@rGO exhibits a superior catalytic activity (∼100 % removal) and robust durability (over ten cycles) in degrading bisphenol A and tetracycline, even in real wastewater scenarios. Furthermore, immobilizing the BiOI@rGO on carbon felt to establish a continuous flow-through device achieves a stable treatment performance with a degradation efficiency exceeding 98 % for micropollutants over a continuous operation. This work provides a paradigm for constructing an acidic microenvironment on the catalyst to surmount the pH limitations of the heterogeneous Fenton reactions for advanced water purification.

摘要

非均相芬顿反应为克服现有均相芬顿工艺中铁污泥积累和可回收性有限的问题提供了机会,但在近中性甚至更高pH条件下其反应活性急剧衰减,仍然是一个巨大的挑战。在这项工作中,我们报道了一种通用且稳健的方法,通过氧化石墨烯键合在BiOI上创建局部酸性微环境,使非均相芬顿(BiOI@rGO/HO)系统能够在较宽的pH范围(3.0 - 10.0)内持续降解有机污染物。值得注意的是,即使在实际废水场景中,BiOI@rGO在降解双酚A和四环素方面也表现出优异的催化活性(约100%去除率)和强大的耐久性(超过十个循环)。此外,将BiOI@rGO固定在碳毡上以建立连续流通装置,在连续运行中对微污染物的降解效率超过98%,实现了稳定的处理性能。这项工作为在催化剂上构建酸性微环境以克服非均相芬顿反应的pH限制用于深度水净化提供了一个范例。

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