Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for efficient water purification

doi:10.1007/s11705-021-2110-6

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (5) : 731-744 https://doi.org/10.1007/s11705-021-2110-6

RESEARCH ARTICLE

Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for efficient water purification

Dean Xu, Tong Ding, Yuqing Sun, Shilong Li, Wenheng Jing(

)

State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China

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Abstract

Catalytic ozonation technology has attracted copious attention in water purification owing to its favorable oxidative degradation of pollutants and mitigation of membrane fouling capacity. However, its extensive industrial application has been restricted by the low ozone utilization and limited mass transfer of the short-lived radical species. Interlayer space-confined catalysis has been theoretically proven to be a viable strategy for achieving high catalytic efficiency. Here, a two-dimensional MnO₂-incorporated ceramic membrane with tunable interspacing, which was obtained via the intercalation of a carbon nanotube, was designed as a catalytic ozonation membrane reactor for degrading methylene blue. Benefiting from the abundant catalytic active sites on the surface of two-dimensional MnO₂ as well as the ultralow mass transfer resistance of fluids due to the nanolayer confinement, an excellent mineralization effect, i.e., 1.2 mg O_3(aq) mg^–1 TOC removal (a total organic carbon removal rate of 71.5%), was achieved within a hydraulic retention time of 0.045 s of pollutant degradation. Further, the effects of hydraulic retention time and interlayer spacing on methylene blue removal were investigated. Moreover, the mechanism of the catalytic ozonation employing catalytic ozonation membrane was proposed based on the contribution of the Mn(III/IV) redox pair to electron transfer to generate the reactive oxygen species. This innovative two-dimensional confinement catalytic ozonation membrane could act as a nanoreactor and separator to efficiently oxidize organic pollutants and enhance the control of membrane fouling during water purification.

Keywords catalytic membrane reactor catalytic ozonation nanoconfinement two-dimensional manganese oxide

Corresponding Author(s): Wenheng Jing

Online First Date: 21 December 2021 Issue Date: 28 March 2022

Cite this article:

Dean Xu,Tong Ding,Yuqing Sun, et al. Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for efficient water purification[J]. Front. Chem. Sci. Eng., 2022, 16(5): 731-744.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-021-2110-6
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I5/731

Fig.1 (a) Photograph of the Tyndall phenomenon. SEM images of the (b) MnO₂ nanosheet powder and (c) and (d) MnO₂ nanosheets that were loaded on the aluminum oxide plate.

Fig.2 (a) Catalytic ozonation of MB by different MnO₂ catalysts; (b) kinetics of the ozonation, as catalyzed by different catalysts (conditions: [MB] = 100 mg·L^–1; pH= original value; [O₃]: 2 mg·L^–1; flow rate= 1 L·min^–1).

Fig.3 (a) Ozone decomposition by different catalysts. Electron paramagnetic resonance (EPR) spectra of the α-MnO₂ nanosheet with (b) DMPO-•OH and (c) DMPO-•O₂⁻. (d) Influence of the radical scavengers on MB removal by α-MnO₂ nanosheet-catalyzed ozonation (conditions: [MB] = 100 mg·L^–1; pH= original value; [O₃]: 2 mg·L^–1; flow rate= 1 L·min^–1; and radical scavengers= 50 mg·L^–1).

Fig.4 Permeability and retention properties of the (a) 2D MnO₂ membrane with different membrane thicknesses, (b) 2D MnO₂-CNT-COM with different CNT loadings, and (c) 2D MnO₂-CNT-COM under different pressure conditions (conditions: [MB] = 10 mg·L^–1; pH= the original value; pressure= 1 bar (a–b)).

Fig.5 O_3(aq) decomposition by different membranes (conditions: [O_3(aq)]: 5 mg·L^–1; pressure= 1 bar).

Fig.6 (a) MB removal by different membranes containing ozone; (b) TOC removal by different membranes with ozone (conditions: [O_3(aq)] = 5 mg·L^–1; [MB] = 10 mg·L^–1; TOC= 6 mg·L^–1; pressure= 1 bar).

Fig.7 MB removals by 2D MnO₂-CNT-COM employing (a) different CNT doping amounts and (b) different pressures (conditions: [O_3(aq)] = 5 mg·L^–1; [MB] = 10 mg·L^–1; pressure= 1 bar (a)).

Fig.8 Self-cleaning performances of 2D MnO₂-CNT-COM/O₃, the modified support/O₃, 2D MnO₂-CNT-COM, and the modified support (conditions: [O_3(aq)] = 5 mg·L^–1; [MB] = 10 mg·L^–1; pressure= 1 bar).

Fig.9 Stability tests for the self-cleaning performance and MB removal of 2D MnO₂-CNT-COM (conditions: [O_3(aq)] = 5 mg·L^–1; [MB] = 10 mg·L^–1; pressure= 1 bar).

Fig.10 Mechanism of MB removal via the confinement-enhanced interface effect of 2D MnO₂-CNT-COM.

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