CuO-OMS-2活化过氧单硫酸盐高效苯酚矿化:性能、活性氧的贡献和催化机制。

IF 5.8 3区 环境科学与生态学 0 ENVIRONMENTAL SCIENCES
Shuang Tian, Jing Liu, Lei Sun, Xiangjuan Yuan, Carme Sans
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引用次数: 0

摘要

本文成功合成了氧化铜负载氧化锰八面体分子筛(CuO-OMS-2)复合材料,并通过过氧单硫酸盐(PMS)活化对苯酚的降解和矿化进行了研究。结果表明,CuO的加入显著促进了多价金属跃迁和氧空位的生成。在初始pH为5.0时,CuO-OMS-2在30 min内达到了最佳的催化活性,苯酚降解效率为93.6%,矿化率为87.6%。此外,建立了基于探针的动力学模型,模拟了不同pH条件下CuO-OMS-2/PMS体系中苯酚的去除,这是影响主要活性自由基转化和氧化能力的决定性因素。活性自由基的定量结果表明,随着pH值从3增加到9,SO4•-的贡献从25.17%逐渐增加到75.60%,而•OH的贡献从69.23%逐渐下降到22.80%。同时,CuO-OMS-2复合材料在连续5次循环中表现出优异的稳定性和可重复使用性。最后,基于探针的动力学模型和表征结果共同验证了CuO-OMS-2活化PMS降解苯酚的机理。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Activation of peroxymonosulfate by CuO-OMS-2 for efficient phenol mineralization: performance, contributions of ROS, and catalytic mechanisms

In this paper, copper oxide supported manganese oxide octahedral molecular sieves (CuO-OMS-2) composite was successfully synthesized and subsequently investigated for the degradation and mineralization of phenol via peroxymonosulfate (PMS) activation. It was confirmed that the incorporation of CuO significantly promoted multivalent metals transition and oxygen vacancies generation. At initial pH 5.0, CuO-OMS-2 achieved the optimum catalytic activity with 93.6% of phenol degradation efficiency and 87.6% of mineralization rate in 30 min. Additionally, a probe-based kinetic model was developed to simulate the removal of phenol in CuO-OMS-2/PMS system under different pH conditions, which was a decisive factor to affect the transformation of main active radicals and the oxidation capacity. The quantitative results of the active radicals suggested that 1O2 and O2•− played generally a negligible role in the abatement of phenol, while the contribution of SO4•− gradually increased from 25.17 to 75.60% and that of OH decreased from 69.23 to 22.80% with the rising of pH from 3 to 9. Meanwhile, the CuO-OMS-2 composite showed excellent stability and reusability for contaminant degradation during five consecutive cycles. Finally, the results of probe-based kinetic model and characterization jointly demonstrated the mechanism of phenol degradation by CuO-OMS-2 activating PMS.

Graphical abstract

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来源期刊
CiteScore
8.70
自引率
17.20%
发文量
6549
审稿时长
3.8 months
期刊介绍: Environmental Science and Pollution Research (ESPR) serves the international community in all areas of Environmental Science and related subjects with emphasis on chemical compounds. This includes: - Terrestrial Biology and Ecology - Aquatic Biology and Ecology - Atmospheric Chemistry - Environmental Microbiology/Biobased Energy Sources - Phytoremediation and Ecosystem Restoration - Environmental Analyses and Monitoring - Assessment of Risks and Interactions of Pollutants in the Environment - Conservation Biology and Sustainable Agriculture - Impact of Chemicals/Pollutants on Human and Animal Health It reports from a broad interdisciplinary outlook.
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