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The in situ catalytic oxidation of sulfamethoxazole via peroxydisufate activation operated in a NG/rGO/CNTs composite membrane filtration

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Abstract

Metal-free carbonaceous composite membranes have been proven to effectively drive novel in situ catalytic oxidation for the degradation of organic pollutants via persulfates activation. In this study, nitrogen-doped graphene (NG) was employed as a modifier to enhance the catalytic activity of the carbon mats by assembly with reduced graphene oxide (rGO) and carbon nanotubes (CNTs) on the top of a nylon supporter. The morphology and performance of the NG/rGO/CNTs composite membrane were compared to those obtained without the addition of NG (rGO/CNTs). Owing to the larger nanochannels for water delivery and stronger hydrophobicity on the surface, the NG/rGO/CNTs composite membrane shows a superior low-pressure filtration performance in favor of energy-saving operation. For the in situ catalytic oxidation of the NG/rGO/CNTs composite membrane through the activation of peroxydisufate (PDS), the average removal rate of sulfamethoxazole (SMX), one of frequently detected sulfonamide antibiotics in water, can reach 21.7 mg·m−2·h−1 under continuous filtration mode, which was 17% more rapid than that of the rGO/CNTs, resulting in significant detoxifying of the oxidation intermediates. Owing to the addition of NG into the carbon mats, the reactive nitrogen-doped sites identified by X-Ray photoelectron spectroscopy (XPS), such as pyridinic and graphitic N, played important roles in PDS activation, while both the radical and non-radical pathways were involved in in situ catalytic oxidation. According to the experimental evidence of the effects that solution environment has on the SMX removal and transmembrane pressure, the NG/rGO/CNTs composite membrane shows a relatively high resistance to changes in the solution pH, chloride ion inhibition, and background organics fouling. These results suggest a new approach to the application of activated persulfate oxidation in water treatment, such that improvements to the reaction stability warrant further investigation.

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Data availability

All data generated or analyzed during this study are included in this published article (and its supplementary information files).

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Acknowledgments

The authors acknowledge the support from the Qinglan Project for Jiangsu Colleges and Universities, China.

Funding

This study was supported by the National Natural Science Foundation of China (51608341), the Natural Science Foundation of Jiangsu Province, China (BK20150284), and the Open Project of National & Local Joint Engineering Laboratory for Municipal Sewage Resource Utilization Technology (No.2019KF02).

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Authors and Affiliations

  1. School of Environmental Science and Engineering, Suzhou University of Science and Technology, No. 1 Kerui Road, Suzhou, 215009, People’s Republic of China

    Feiyue Qian, Honggui Yin, Feng Liu, Jiayi Sheng, Shiqian Gao & Yaoliang Shen

  2. National and Local Joint Engineering Laboratory of Municipal Sewage Resource Utilization Technology, No. 1 Kerui Road, Suzhou, 215009, People’s Republic of China

    Feiyue Qian, Feng Liu, Shiqian Gao & Yaoliang Shen

Authors
  1. Feiyue Qian
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  2. Honggui Yin
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  3. Feng Liu
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  4. Jiayi Sheng
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  5. Shiqian Gao
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  6. Yaoliang Shen
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Contributions

Feiyue Qian developed the research proposal, and was a major contributor in writing the manuscript; Honggui Yin and Jiayi Sheng performed the fabrication of composite membranes and in situ catalytic oxidation for SMX degradation, analyzed the original experiment data; Shiqian Gao developed the quantitative analysis methods of SMX at low concentration, and was responsible for the extraction of oxidation intermediates from the filtrate. Feng Liu designed the system of in situ catalytic oxidation, and interpreted the results regarding the effects of solution environment; Yaoliang Shen gave important suggestions in the improvement of this manuscript. All authors read and approved the final manuscript.

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Correspondence to Feiyue Qian.

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Qian, F., Yin, H., Liu, F. et al. The in situ catalytic oxidation of sulfamethoxazole via peroxydisufate activation operated in a NG/rGO/CNTs composite membrane filtration. Environ Sci Pollut Res 28, 26828–26839 (2021). https://doi.org/10.1007/s11356-021-12545-1

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