铜掺杂氧化锰八面体分子筛的制备及其高效降解磺胺甲恶唑性能研究

邱宇华; 黄应平; 王燕兰; 刘湘; 黄笛

doi:10.1007/s12613-024-2858-z

Volume 31 Issue 12

Dec. 2024

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文章导航 > 矿物冶金与材料学报（英文） > 2024 > 31(12): 2770-2780

Yuhua Qiu, Yingping Huang, Yanlan Wang, Xiang Liu, and Di Huang, Facile synthesis of Cu-doped manganese oxide octahedral molecular sieve for the efficient degradation of sulfamethoxazole via peroxymonosulfate activation, Int. J. Miner. Metall. Mater., 31(2024), No. 12, pp. 2770-2780. https://doi.org/10.1007/s12613-024-2858-z

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Yuhua Qiu, Yingping Huang, Yanlan Wang, Xiang Liu, and Di Huang, Facile synthesis of Cu-doped manganese oxide octahedral molecular sieve for the efficient degradation of sulfamethoxazole via peroxymonosulfate activation, Int. J. Miner. Metall. Mater., 31(2024), No. 12, pp. 2770-2780. https://doi.org/10.1007/s12613-024-2858-z

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研究论文

铜掺杂氧化锰八面体分子筛的制备及其高效降解磺胺甲恶唑性能研究

1)
三峡大学材料与化学工程学院, 三峡库区生态环境教育部工程研究中心, 宜昌443002
2)
聊城大学化学化工学院, 聊城 252059

通讯作者:
刘湘 E-mail: xiang.liu@ctgu.edu.cn

黄笛 E-mail: huangd94@iccas.ac.cn

文章亮点

(1) 通过在氧化锰八面体分子筛(OMS-2)中掺杂Cu元素，合成了Cu-OMS-2纳米棒，显著增强OMS-2的活性。

(2) 研究了Cu-OMS-2纳米棒活化PMS高效降解SMX的机理。

(3) 展示了Cu-OMS-2/PMS在污水处理的潜在应用前景。

中文摘要

以过氧单硫酸根(PMS)为基础的高级氧化法是去除污水中有毒和难降解有机污染物的有效方法。活化吸电子的$ {\mathrm{H}\mathrm{S}\mathrm{O}}_{5}^{-} $释放出硫酸盐自由基($ {\text{·}\mathrm{S}\mathrm{O}}_{4}^{-} $)、羟基自由基($ \text{·}\mathrm{O}\mathrm{H} $)、超氧自由基($ {\text{·}\mathrm{O}}_{2}^{-} $)和单线态氧(¹O₂)等活性物质，可诱导有机污染物的降解。本研究通过在氧化锰八面体分子筛(OMS-2)中掺杂Co²⁺、Ni²⁺、Cu²⁺、Fe³⁺，合成了多种M-OMS-2纳米棒(M = Co、Ni、Cu、Fe)，通过活化PMS高效去除磺胺甲恶唑(SMX)。考察了M-OMS-2活化PMS去除SMX的催化性能。SMX去除率由高到低依次为Cu-OMS-2(96.40%) > Co-OMS-2(88.00%) > Ni-OMS-2(87.20%) > Fe-OMS-2(35.00%) > OMS-2(33.50%)。然后，研究了M-OMS-2纳米棒在去除SMX过程中的动力学和构效关系。通过猝灭实验、高分辨率质谱和电子顺磁共进一步研究了Cu-OMS-2/PMS体系降解SMX的可行机制。结果表明: Cu-OMS-2/PMS系统在海水和自来水中对SMX的降解效率均有提高，显示了该系统在污水处理中的潜在应用前景。

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Research Article

Facile synthesis of Cu-doped manganese oxide octahedral molecular sieve for the efficient degradation of sulfamethoxazole via peroxymonosulfate activation

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Abstract

Abstract

Advanced processes for peroxymonosulfate (PMS)-based oxidation are efficient in eliminating toxic and refractory organic pollutants from sewage. The activation of electron-withdrawing $ {\mathrm{HSO}}_{5}^{-} $ releases reactive species, including sulfate radical ($ {\text{·}\mathrm{S}\mathrm{O}}_{4}^{-} $), hydroxyl radical ($ \text{·}\mathrm{O}\mathrm{H} $), superoxide radical ($ {\text{·}\mathrm{O}}_{2}^{-} $), and singlet oxygen (¹O₂), which can induce the degradation of organic contaminants. In this work, we synthesized a variety of M-OMS-2 nanorods (M = Co, Ni, Cu, Fe) by doping Co²⁺, Ni²⁺, Cu²⁺, or Fe³⁺ into manganese oxide octahedral molecular sieve (OMS-2) to efficiently remove sulfamethoxazole (SMX) via PMS activation. The catalytic performance of M-OMS-2 in SMX elimination via PMS activation was assessed. The nanorods obtained in decreasing order of SMX removal rate were Cu-OMS-2 (96.40%), Co-OMS-2 (88.00%), Ni-OMS-2 (87.20%), Fe-OMS-2 (35.00%), and OMS-2 (33.50%). Then, the kinetics and structure–activity relationship of the M-OMS-2 nanorods during the elimination of SMX were investigated. The feasible mechanism underlying SMX degradation by the Cu-OMS-2/PMS system was further investigated with a quenching experiment, high-resolution mass spectroscopy, and electron paramagnetic resonance. Results showed that SMX degradation efficiency was enhanced in seawater and tap water, demonstrating the potential application of Cu-OMS-2/PMS system in sewage treatment.
- sulfamethoxazole;
- manganese oxide octahedral molecular sieve;
- peroxymonosulfate;
- sewage treatment;
- copper

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铜掺杂氧化锰八面体分子筛的制备及其高效降解磺胺甲恶唑性能研究

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Facile synthesis of Cu-doped manganese oxide octahedral molecular sieve for the efficient degradation of sulfamethoxazole via peroxymonosulfate activation

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