Nanoconfined Cobalt Ferrite Composite Carbon Nanotube Membrane Oxidation-Filtration System for Water Decontamination

IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL ACS ES&T engineering Pub Date : 2024-08-12 DOI:10.1021/acsestengg.4c00282
Huanran Ma, Lijun Zhang, Xiao Zhang, Zonglin Pan, Ruisong Xu, Guanlong Wang, Xinfei Fan, Huixia Lu, Shuaifei Zhao, Chengwen Song
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Abstract

Constructing a membrane-confined peroxymonosulfate (PMS) activation system has emerged as a promising strategy for efficient water decontamination. Herein, a novel cobalt ferrite (CoFe2O4)-filled open-end carbon nanotube (OCNT) membrane filtration system was proposed, aiming to integrate dual metal centers and nanoconfinement for enhancing PMS activation (MFPA) toward water decontamination. The optimal CoFe2O4@OCNT MFPA process displayed 100% phenol removal within a residence time of 5.7 s, whose k (1.17 s–1) was 3.0, 5.6, and 3.9 times higher than that of CoO@OCNT, FeO@OCNT, and CoFe2O4/CCNT (surface-loaded closed end cap CNT), respectively. Experimental results and theoretical calculations jointly unravel the nonradical-dominated (1O2 and electron transfer) oxidation mechanism, leading to the wide-pH adaptation and superior stability in the complex water matrix. Mechanism analysis showed that fast cycling of Co2+/Co3+ was achieved via synergistic promotion between dual metal centers and the nanoconfinement effect, which coboosted the PMS consumption as well as reactive oxygen species generation (especially 1O2). Compared with the single metal center, the dual metal centers of internal CoFe2O4 exhibited coenhanced electron cloud density (amount of charge transfer) and adsorption energy for PMS, resulting in O–O cleavage and elongated O–H. Meanwhile, the oxygen vacancy defect (Odef) on CoFe2O4 also contributed to the nonradical process, which not only served as the precursor of 1O2 generation but also acted as a transfer station for electrons.

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用于水净化的纳米钴铁氧体复合碳纳米管膜氧化-过滤系统
构建膜封闭式过一硫酸盐(PMS)活化系统已成为一种很有前途的高效水净化策略。本文提出了一种新型的铁氧体钴(CoFe2O4)填充开口碳纳米管(OCNT)膜过滤系统,旨在整合双金属中心和纳米细化技术,以增强过硫酸盐活化(MFPA),从而达到净化水的目的。最佳的 CoFe2O4@OCNT MFPA 工艺在 5.7 秒的停留时间内实现了 100% 的苯酚去除率,其 k 值(1.17 s-1)分别是 CoO@OCNT、FeO@OCNT 和 CoFe2O4/CCNT(表面负载封闭端盖 CNT)的 3.0、5.6 和 3.9 倍。实验结果和理论计算共同揭示了非自由基主导(1O2 和电子传递)的氧化机理,从而使其在复杂的水基质中具有较宽的 pH 适应性和优异的稳定性。机理分析表明,Co2+/Co3+ 的快速循环是通过双金属中心之间的协同促进作用和纳米融合效应实现的,这共同促进了 PMS 的消耗和活性氧(尤其是 1O2)的生成。与单金属中心相比,内部 CoFe2O4 的双金属中心表现出共同增强的电子云密度(电荷转移量)和对 PMS 的吸附能,从而导致 O-O 裂解和 O-H 拉伸。同时,CoFe2O4 上的氧空位缺陷(Odef)也促进了非辐射过程,它不仅是生成 1O2 的前体,也是电子的中转站。
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来源期刊
ACS ES&T engineering
ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-
CiteScore
8.50
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0.00%
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0
期刊介绍: ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources. The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope. Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.
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