Unraveling the time evolution and post mortem changes of nanometric MnOOH during in situ oxidation of ciprofloxacin by activated peroxymonosulfate

IF 21.1 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-06-15 DOI:10.1016/j.apcatb.2023.122439

Yeison Núñez-de la Rosa , Luis Guillermo Cuadrado Durango , Moacir Rossi Forim , Otaciro Rangel Nascimento , Peter Hammer , José M. Aquino

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引用次数: 3

Abstract

Nanometric MnOOH compound was synthesized by a green approach, characterized, and used to remove ciprofloxacin (CIP) antibiotic by in situ chemical oxidation using peroxymonosulfate (PMS). The effects of varying concentrations of MnOOH, PMS and pH, on morphological, structural, chemical, and electrochemical changes were studied during and after the experiments. The CIP molecule was completely oxidized and partially mineralized (>60%) after 6 h under acidic conditions. The mechanism of CIP degradation was induced by PMS activated oxidants (HO^• and ¹O₂) and, to a lesser extent, directly on the surface of MnOOH. The latter process was evidenced by transmission electron microscopy showing the formation of an amorphous shell (MnO₂) over MnOOH crystallites, as verified using X-ray photoelectron spectroscopy and the subsequent increase of the charge transfer resistance that hindered a further electron transfer to the PMS oxidant. Such behavior is recoverable when using a freshly prepared PMS solution.

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揭示了活化过氧单硫酸根原位氧化环丙沙星过程中纳米MnOOH的时间演变和死后变化

采用绿色方法合成了纳米MnOOH化合物，对其进行了表征，并将其用于过氧单硫酸根(PMS)原位化学氧化去除环丙沙星(CIP)抗生素。研究了不同浓度的MnOOH、PMS和pH对实验期间和实验结束后形貌、结构、化学和电化学变化的影响。在酸性条件下6 h后，CIP分子被完全氧化，部分矿化(60%)。CIP的降解机制是由PMS活化的氧化剂(HO•和1O2)诱导的，在较小程度上直接作用于MnOOH表面。后一过程通过透射电子显微镜证实，在MnOOH晶体上形成了一个无定形壳层(MnO2)，用x射线光电子能谱证实了这一点，随后电荷转移电阻的增加阻碍了电子进一步转移到PMS氧化剂。当使用新配制的PMS溶液时，这种行为是可恢复的。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.