Diatomic "catalytic/co-catalytic" Fe/Mo catalysts promote Fenton-like reaction to treat organic wastewater through special interfacial reaction enhancement mechanism

IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Zhen Liu , Xin-Yi Xu , Fei Xu , Rui-Dian Su , Bin Li , Fang Zhang , Xing Xu , Yan Wang , De-Fang Ma , Bao-Yu Gao , Qian Li
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Abstract

The full utilization of active sites and the effective Fe2+/Fe3+cycling are the key problems that expand the application of iron-based Fenton-like reaction in water purification. In this paper, a novel diatomic Fe/Mo catalyst (Fe/Mo-DACs) was used to enhance the interfacial reaction mechanism with oxidant to achieve more stronger selective degradation of electron-donating organic pollutants. The availability of Fe sites during the activation of peroxymonosulfate (PMS) was enhanced by the adjacent atomic Mo sites, and the resulting special interfacial complex (Fe/Mo-DACs-PMS*) possessed higher activity, stability and selectivity (especially for electron-donating organics). The degradation rate of bisphenol A (BPA) in Fe/Mo-DACs/PMS system (0.642 min-1) was increased by two times compared with the corresponding Fe single-atomic reaction system. Density functional theory calculation analysis further indicated that the diatomic Fe/Mo site was the true activation center of PMS, and other independent single-atom Fe sites cooperated to optimize the interface reaction mechanism (adsorption and activation) of PMS on the materials’ surface. Moreover, the promotion of Fe2+/Fe3+ cycling by Mo sites further enhanced the sustainability and adaptability of this degradation system. The atomic-level "catalytic/co-catalytic" materials are expected to broaden the design idea of heterogeneous materials and enhance the application prospect of Fenton-like reactions in water pollution control.

Abstract Image

Abstract Image

二原子 "催化/共催化 "铁/钼催化剂通过特殊的界面反应增强机制促进类似芬顿的反应,以处理有机废水
活性位点的充分利用和Fe2+/Fe3+的有效循环是扩大铁基类芬顿反应在水净化中的应用的关键问题。本文采用一种新型双原子Fe/Mo催化剂(Fe/Mo- dac),增强了其与氧化剂的界面反应机制,实现了对供电子有机污染物更强的选择性降解。在过氧单硫酸盐(PMS)活化过程中,相邻的原子Mo位点增强了Fe位点的可用性,形成的特殊界面配合物(Fe/Mo- dac -PMS*)具有更高的活性、稳定性和选择性(特别是对供电子有机物)。双酚A (BPA)在Fe/ mo - dac /PMS体系中的降解速率(0.642 min-1)比相应的Fe单原子反应体系提高了2倍。密度泛函理论计算分析进一步表明,双原子Fe/Mo位点是PMS的真正活化中心,其他独立的单原子Fe位点协同作用优化了PMS在材料表面的界面反应机理(吸附和活化)。此外,Mo位点对Fe2+/Fe3+循环的促进进一步增强了该降解系统的可持续性和适应性。原子级“催化/共催化”材料有望拓宽非均相材料的设计思路,增强类芬顿反应在水污染控制中的应用前景。
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来源期刊
Water Research
Water Research 环境科学-工程:环境
CiteScore
20.80
自引率
9.40%
发文量
1307
审稿时长
38 days
期刊介绍: Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.
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