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

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.

Key words： catalytic membrane reactor; catalytic ozonation; nanoconfinement; two-dimensional manganese oxide

Acknowledgments

This study was financially supported by the National Natural Science Foundation of China (Grant Nos. 21838005 and 21676139) and the Key Scientific Research and Development Projects of Jiangsu Province (Grant No. BE201800901). The authors would like to thank Shiyanjia Laboratory for the language editing service.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://dx.doi.org/10.1007/s11705-021-2110-6 and is accessible for authorized users.

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