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

doi:10.1007/s11783-023-1706-0

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (9) : 106 https://doi.org/10.1007/s11783-023-1706-0

RESEARCH ARTICLE

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

Xufang Wang¹, Dongli Guo¹, Jinna Zhang², Yuan Yao³(

), Yanbiao Liu^1,⁴(

)

¹. College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
². State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China
³. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150080, China
⁴. Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China

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Abstract

● 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.

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.

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

Corresponding Author(s): Yuan Yao,Yanbiao Liu

Issue Date: 31 March 2023

Cite this article:

Xufang Wang,Dongli Guo,Jinna Zhang, et al. Insights into the electron transfer mechanisms of permanganate activation by carbon nanotube membrane for enhanced micropollutants degradation[J]. Front. Environ. Sci. Eng., 2023, 17(9): 106.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1706-0
https://academic.hep.com.cn/fese/EN/Y2023/V17/I9/106

Fig.1 SMX oxidation flux under different KMnO₄ concentrations in the (a) KMnO₄ alone system and (b) CNT/KMnO₄ system. Experimental conditions: [SMX]₀ = 80 μmol/L, flow rate = 0.5 mL/min, and pH = 6.2.

Fig.2 (a) The effect of PMSO on SMX oxidation in the CNT/KMnO₄ system, (b) UV-visible spectrum of different solution samples, (c) SMX oxidation in various systems, (d) UV-visible spectrum of different solution samples in the presence of 1.0 mmol/L pyrophosphate. Experimental conditions: [SMX]₀ = 80 μmol/L, [KMnO₄]₀ = 1.0 mmol/L, flow rate = 0.5 mL/min, and pH = 6.2.

Fig.3 XPS spectra of CNT: (a) survey spectrum, core-level spectra of (b) Mn 2p and (c) O 1s.

Fig.4 (a) Chronoamperometry in 50 mmol/L Na₂SO₄ electrolyte solution at Pt electrodes and (b) proposed mechanisms of SMX oxidation in the CNT/KMnO₄ system.

Fig.5 The potential difference in molecular orbitals drives electron transmission via the structural defects of CNT.

Fig.6 (a) The schematic illustration of the KMnO₄/CNT system, and (b) the stability analysis for SMX oxidation flux. Experimental conditions: [SMX]₀ = 80 μmol/L, [KMnO₄]₀ = 1.0 mmol/L, flow rate = 0.5 mL/min, and pH = 6.2.

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