Insights into the electron transfer mechanisms of permanganate activation by carbon nanotube membrane for enhanced micropollutants degradation

Highlights

● A CNT filter enabled effective KMnO₄ activation via facilitated electron transfer.

● Ultra-fast degradation of micropollutants were achieved in KMnO₄/CNT system.

● CNT mediated electron transfer process from electron-rich molecules to KMnO₄.

● Electron transfer dominated organic degradation.

Abstract

Numerous reagents have been proposed as electron sacrificers to induce the decomposition of permanganate (KMnO₄) by producing highly reactive Mn species for micropollutants degradation. However, this strategy can lead to low KMnO₄ utilization efficiency due to limitations associated with poor mass transport and high energy consumption. In the present study, we rationally designed a catalytic carbon nanotube (CNT) membrane for KMnO₄ activation toward enhanced degradation of micropollutants. The proposed flow-through system outperformed conventional batch reactor owing to the improved mass transfer via convection. Under optimal conditionals, a > 70% removal (equivalent to an oxidation flux of 2.43 mmol/(h·m²)) of 80 μmol/L sulfamethoxazole (SMX) solution can be achieved at single-pass mode. The experimental analysis and DFT studies verified that CNT could mediate direct electron transfer from organic molecules to KMnO₄, resulting in a high utilization efficiency of KMnO₄. Furthermore, the KMnO₄/CNT system had outstanding reusability and CNT could maintain a long-lasting reactivity, which served as a green strategy for the remediation of micropollutants in a sustainable manner. This study provides new insights into the electron transfer mechanisms and unveils the advantages of effective KMnO₄ utilization in the KMnO₄/CNT system for environmental remediation.

Graphical abstract

Keywords

KMnO₄ / Carbon nanotubes / Non-radical pathway / Electron transfer / Water treatment

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Acknowledgements

This work was financially supported by the Natural Science Foundation of Shanghai (No. 23ZR1401300) and the National Natural Science Foundation of China (No. 52170068).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-023-1706-0 and is accessible for authorized users.

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