通过Fe2O3/VO2双金属催化剂的双重氧化还原循环增强PMS活性,有效降解SCP

IF 6.7 2区 工程技术 Q1 ENGINEERING, CHEMICAL
YaGe Chai , Qiongfang Wang , Xin Zhang , Lei Dong , Min Zhang , Pinhua Rao , Naiyun Gao
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引用次数: 0

摘要

在本研究中,通过引入V,成功制备双金属催化剂Fe2O3/VO2,可以解决Fe2+/ Fe3+氧化还原循环引起的Fe2O3在过氧单硫酸盐(PMS)活化过程中的活性限制。采用溶剂热法合成Fe2O3/VO2,调节Fe/V摩尔比(X = 1,2,3),其中Fe/V摩尔比为2:1的最佳Fe/V比显示出优异的PMS活性,可以有效地降解磺胺氯吡啶(SCP)。Fe2O3/VO2/PMS体系在较宽的pH范围内(3-9)表现出优异的催化性能,在0.25 mM PMS下在10分钟内完全降解SCP。阴离子(Cl−、NO₃−、H₂PO₄−、HPO₄2−、HCO₃−)和腐植酸对SCP的氧化有不同程度的抑制作用。Fe2O3/VO2催化体系通过Fe2+/ V4+的电子转移激活PMS,同时启动自由基(SO4−和OH)和非自由基(主要是1O2)途径,其协同作用使污染物降解效率高。这些活性氧的协同作用促进了抗生素的有效降解,其中1O2被认为是主要的活性物质。利用HPLC-MS鉴定了13个中间产物,并提出了3种降解途径。生态毒性评价表明,大多数中间体的毒性明显低于SCP,证实了Fe2O3/VO2/PMS系统在废水修复中的潜力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Enhanced PMS activation via dual redox cycles in Fe2O3/VO2 bimetallic catalyst for efficient degradation of SCP
In this study, limitation of Fe2O3 activity in peroxymonosulfate (PMS) activation processes caused by the Fe2+/ Fe3+ redox cycle could be addressed by successfully preparing the bimetallic catalyst Fe2O3/VO2 with introducing V. Fe2O3/VO2 were synthesized using a solvothermal method and Fe/V molar ratios (X = 1, 2, 3) were regulated, in which optimal Fe/V ratio of 2:1 demonstrated superior PMS activation to efficiently degrade sulfachloropyridazine (SCP). The Fe2O3/VO2/PMS system exhibited excellent catalytic performance across a wide pH range (3–9), achieving complete degradation of SCP with 0.25 mM PMS in 10 min. Anions (Cl, NO₃, H₂PO₄, HPO₄2−, HCO₃) and humic acid showed varying inhibitory effects on SCP oxidation. The Fe2O3/VO2 catalytic system activates PMS through electron transfer from Fe2+/ V4+, simultaneously initiating both radical (SO4 and OH) and non-radical (primarily 1O2) pathways, whose synergistic effect enables highly efficient pollutant degradation. The synergistic effects of these ROS facilitated efficient antibiotic degradation, with 1O2 identified as the primary active species. Using HPLC-MS, 13 intermediate products were identified, and three degradation pathways were proposed. Ecotoxicity assessment indicated that most intermediates were significantly less toxic than SCP, confirming the Fe2O3/VO2/PMS system's potential for wastewater remediation.
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来源期刊
Journal of water process engineering
Journal of water process engineering Biochemistry, Genetics and Molecular Biology-Biotechnology
CiteScore
10.70
自引率
8.60%
发文量
846
审稿时长
24 days
期刊介绍: The Journal of Water Process Engineering aims to publish refereed, high-quality research papers with significant novelty and impact in all areas of the engineering of water and wastewater processing . Papers on advanced and novel treatment processes and technologies are particularly welcome. The Journal considers papers in areas such as nanotechnology and biotechnology applications in water, novel oxidation and separation processes, membrane processes (except those for desalination) , catalytic processes for the removal of water contaminants, sustainable processes, water reuse and recycling, water use and wastewater minimization, integrated/hybrid technology, process modeling of water treatment and novel treatment processes. Submissions on the subject of adsorbents, including standard measurements of adsorption kinetics and equilibrium will only be considered if there is a genuine case for novelty and contribution, for example highly novel, sustainable adsorbents and their use: papers on activated carbon-type materials derived from natural matter, or surfactant-modified clays and related minerals, would not fulfil this criterion. The Journal particularly welcomes contributions involving environmentally, economically and socially sustainable technology for water treatment, including those which are energy-efficient, with minimal or no chemical consumption, and capable of water recycling and reuse that minimizes the direct disposal of wastewater to the aquatic environment. Papers that describe novel ideas for solving issues related to water quality and availability are also welcome, as are those that show the transfer of techniques from other disciplines. The Journal will consider papers dealing with processes for various water matrices including drinking water (except desalination), domestic, urban and industrial wastewaters, in addition to their residues. It is expected that the journal will be of particular relevance to chemical and process engineers working in the field. The Journal welcomes Full Text papers, Short Communications, State-of-the-Art Reviews and Letters to Editors and Case Studies
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