热解硝基三乙酸-锰/铁生成 MnFe2O4/C 纳米粒子:活化高碘酸盐降解有机污染物的优异性能

IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Process Safety and Environmental Protection Pub Date : 2024-11-15 DOI:10.1016/j.psep.2024.11.030
Li Chen, Yingchun Yang, Wenjing Tang, Haolan Huang
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引用次数: 0

摘要

四环素(TC)的滥用可能会导致环境风险,对人类健康造成危害。高级氧化工艺(AOPs)可以产生高活性自由基,从而有效降解污染物。高碘酸盐(PI)因其优异的氧化性能,在 AOPs 中受到越来越多的关注。为了提高污染物的降解效率,硝基三乙酸(NTA)与铁和锰形成络合物,然后通过热解成功合成了 MnFe2O4/C,以活化 PI。研究了催化剂用量、PI 浓度和 pH 值。在最佳条件下(催化剂 = 200 mg/L、PI = 500 mg/L、pH = 4.0),60 分钟后 TC 的降解效率达到 94.0%。MnFe2O4/C 卓越的 PI 活化性能得益于 Mn3+/Mn2+ 和 Fe3+/Fe2+ 的氧化还原循环。通过淬灭实验证明,碘自由基(IO3-)是 TC 降解的主要活性物种。此外,SO42、Cl、CO32、HCO3、NO3 和腐殖酸(HA)对该体系中 TC 的降解效率影响不大。最后,通过高效液相色谱-质谱(HPLC-MS)和密度泛函理论(DFT)提出了 TC 的降解途径。中间产物没有严重毒性,也没有产生有毒的碘物种(I2、I3、HOI)。总体而言,该研究在降解污染物的过程中没有产生有毒物质,安全环保。
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Pyrolysis of nitrilotriacetic acid-Mn/Fe to produce MnFe2O4/C nanoparticles: Excellent performance of activating periodate to degrade organic pollutants
The abuse of tetracycline (TC) may lead to environmental risks and cause harm to human health. Advanced oxidation process (AOPs) can produce highly reactive free radicals, which can effectively degrade pollutants. Periodate (PI) has received more attention in AOPs due to its excellent oxidation property. To improve the degradation efficiency of pollutants, nitrilotriacetic acid (NTA) formed complexes with Fe and Mn, then MnFe2O4/C was successfully synthesized by pyrolysis to activate PI. The catalyst dosage, PI concentration, and pH values were investigated. Under optimal conditions (catalyst = 200 mg/L, PI = 500 mg/L, and pH = 4.0), the degradation efficiency of TC reached 94.0 % at 60 min. The excellent PI activation performance of MnFe2O4/C was attributed to the redox cycle of Mn3+/Mn2+ and Fe3+/Fe2+. Through quenching experiments, it has been demonstrated that iodine radical (IO3) was the main active species for TC degradation. Furthermore, the degradation efficiency of TC in this system was not seriously affected by SO42, Cl, CO32, HCO3, NO3, and humic acid (HA). Finally, the degradation pathways of TC were proposed by high performance liquid chromatography mass (HPLC-MS) and density functional theory (DFT). The intermediates were not seriously toxic, and no toxic iodine species (I2, I3, HOI) were produced. Overall, this study did not generate toxic substances in the process of degradation of pollutants, which is safe and environmentally friendly.
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来源期刊
Process Safety and Environmental Protection
Process Safety and Environmental Protection 环境科学-工程:化工
CiteScore
11.40
自引率
15.40%
发文量
929
审稿时长
8.0 months
期刊介绍: The Process Safety and Environmental Protection (PSEP) journal is a leading international publication that focuses on the publication of high-quality, original research papers in the field of engineering, specifically those related to the safety of industrial processes and environmental protection. The journal encourages submissions that present new developments in safety and environmental aspects, particularly those that show how research findings can be applied in process engineering design and practice. PSEP is particularly interested in research that brings fresh perspectives to established engineering principles, identifies unsolved problems, or suggests directions for future research. The journal also values contributions that push the boundaries of traditional engineering and welcomes multidisciplinary papers. PSEP's articles are abstracted and indexed by a range of databases and services, which helps to ensure that the journal's research is accessible and recognized in the academic and professional communities. These databases include ANTE, Chemical Abstracts, Chemical Hazards in Industry, Current Contents, Elsevier Engineering Information database, Pascal Francis, Web of Science, Scopus, Engineering Information Database EnCompass LIT (Elsevier), and INSPEC. This wide coverage facilitates the dissemination of the journal's content to a global audience interested in process safety and environmental engineering.
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