{"title":"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","authors":"Huanran Ma, Lijun Zhang, Xiao Zhang, Zonglin Pan, Ruisong Xu, Guanlong Wang, Xinfei Fan, Huixia Lu, Shuaifei Zhao, Chengwen Song","doi":"10.1021/acsestengg.4c00282","DOIUrl":null,"url":null,"abstract":"Constructing a membrane-confined peroxymonosulfate (PMS) activation system has emerged as a promising strategy for efficient water decontamination. Herein, a novel cobalt ferrite (CoFe<sub>2</sub>O<sub>4</sub>)-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 CoFe<sub>2</sub>O<sub>4</sub>@OCNT MFPA process displayed 100% phenol removal within a residence time of 5.7 s, whose <i>k</i> (1.17 s<sup>–1</sup>) was 3.0, 5.6, and 3.9 times higher than that of CoO@OCNT, FeO@OCNT, and CoFe<sub>2</sub>O<sub>4</sub>/CCNT (surface-loaded closed end cap CNT), respectively. Experimental results and theoretical calculations jointly unravel the nonradical-dominated (<sup>1</sup>O<sub>2</sub> 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 Co<sup>2+</sup>/Co<sup>3+</sup> 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 <sup>1</sup>O<sub>2</sub>). Compared with the single metal center, the dual metal centers of internal CoFe<sub>2</sub>O<sub>4</sub> 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 (O<sub>def</sub>) on CoFe<sub>2</sub>O<sub>4</sub> also contributed to the nonradical process, which not only served as the precursor of <sup>1</sup>O<sub>2</sub> generation but also acted as a transfer station for electrons.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Nanoconfined Cobalt Ferrite Composite Carbon Nanotube Membrane Oxidation-Filtration System for Water Decontamination\",\"authors\":\"Huanran Ma, Lijun Zhang, Xiao Zhang, Zonglin Pan, Ruisong Xu, Guanlong Wang, Xinfei Fan, Huixia Lu, Shuaifei Zhao, Chengwen Song\",\"doi\":\"10.1021/acsestengg.4c00282\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Constructing a membrane-confined peroxymonosulfate (PMS) activation system has emerged as a promising strategy for efficient water decontamination. Herein, a novel cobalt ferrite (CoFe<sub>2</sub>O<sub>4</sub>)-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 CoFe<sub>2</sub>O<sub>4</sub>@OCNT MFPA process displayed 100% phenol removal within a residence time of 5.7 s, whose <i>k</i> (1.17 s<sup>–1</sup>) was 3.0, 5.6, and 3.9 times higher than that of CoO@OCNT, FeO@OCNT, and CoFe<sub>2</sub>O<sub>4</sub>/CCNT (surface-loaded closed end cap CNT), respectively. Experimental results and theoretical calculations jointly unravel the nonradical-dominated (<sup>1</sup>O<sub>2</sub> 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 Co<sup>2+</sup>/Co<sup>3+</sup> 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 <sup>1</sup>O<sub>2</sub>). Compared with the single metal center, the dual metal centers of internal CoFe<sub>2</sub>O<sub>4</sub> 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 (O<sub>def</sub>) on CoFe<sub>2</sub>O<sub>4</sub> also contributed to the nonradical process, which not only served as the precursor of <sup>1</sup>O<sub>2</sub> generation but also acted as a transfer station for electrons.\",\"PeriodicalId\":7008,\"journal\":{\"name\":\"ACS ES&T engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2024-08-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS ES&T engineering\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1021/acsestengg.4c00282\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS ES&T engineering","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1021/acsestengg.4c00282","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Nanoconfined Cobalt Ferrite Composite Carbon Nanotube Membrane Oxidation-Filtration System for Water Decontamination
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.
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.