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Refractory organic compounds in coal chemical wastewater treatment by catalytic ozonation using Mn-Cu-Ce/Al2O3

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Abstract

A composite Mn-Cu-Ce tri-metal oxide supported on γ-Al2O3 (Mn-Cu-Ce/Al2O3) catalyst was prepared by an impregnation-calcination method and investigated in the catalytic ozonation treatment of real coal chemical wastewater (CCW). The catalyst was characterized by XRD, SEM, TEM, XRF, BET, and XPS techniques. The results showed that Mn, Cu, and Ce metal oxides were evenly distributed on the Al2O3 surface and the catalyst maintained a large surface area and a high pore volume compared with the pristine Al2O3. The synergy between Mn, Cu, and Ce oxides greatly enriched the catalytic active sites and enhanced the ozonation performance. The catalytic ozonation process with Mn-Cu-Ce/Al2O3 increased the removal rate of total organic carbon (TOC) by 31.6% compared with ozonation alone. The ketones, aromatic compounds, phenols, and nitrogen-containing heterocyclic compounds in CCW have been effectively degraded and mineralized by Mn-Cu-Ce/Al2O3 catalytic ozonation process, and its biodegradability has also been significantly improved. The experimental results of ∙OH scavengers revealed that the mechanism of Mn-Cu-Ce/Al2O3 catalytic ozonation was to promote the generation of ∙OH radicals. The catalytic activity of Mn-Cu-Ce/Al2O3 was only a slight decrease in six consecutive catalytic ozonation treatments, showing good stability. Therefore, Mn-Cu-Ce/Al2O3 can be used as a candidate catalyst for the advanced treatment of refractory organic wastewaters upon catalytic ozonation.

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The datasets used and analyzed during the current study can be obtained from the corresponding author upon reasonable request.

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Acknowledgements

The authors sincerely acknowledge the Test and Analysis Center of Ningxia University for providing analysis equipment for this research.

Funding

This project was financially supported by The East-West Cooperation Project of Ningxia Key R&D Plan (2017BY064), Project of Ningxia Key R&D Plan (2020YCZX), and National First-rate Discipline Construction Project of Ningxia (NXYLXK2017A04).

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ZKH was responsible for conducting the experiment and writing the manuscript. LF and GSY analyzed the experimental results. ZL revised the manuscript. MYL directed the research, acquired funding, and reviewed the manuscript. All authors contributed to the analysis and writing of the manuscript.

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Correspondence to Yu-Long Ma.

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Zhao, KH., Ma, YL., Lin, F. et al. Refractory organic compounds in coal chemical wastewater treatment by catalytic ozonation using Mn-Cu-Ce/Al2O3. Environ Sci Pollut Res 28, 41504–41515 (2021). https://doi.org/10.1007/s11356-021-13629-8

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  • DOI: https://doi.org/10.1007/s11356-021-13629-8

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