Efficient activation of peroxymonosulfate by sulfur-coordinated iron-based two-dimensional composite membrane (S-Fe@G) via sulfur doping and nanoconfined catalysis
File(s)
Accepted version
Author(s)
Type
Journal Article
Abstract
The combination of nanoconfined catalysis, sulfate radicals based-advanced oxidation processes (SR-AOPs) and membrane filtration processes, can remove organic pollutants efficiently while eliminating the need for secondary recovery of heterogeneous catalysts. In this study, sulfur-doped iron-based carbonaceous two-dimensional composite nanoconfined catalytic membranes (S–Fe@G membranes) were prepared to rapidly activate peroxymonosulfate (PMS) for efficient water purification. The best performing 2S–20Fe@G catalytic membrane/PMS system achieved an ultra-rapid (158.7 ms retention time) removal (94.9 %) and high mineralization (>66.7 %) of tetracycline (TC, 20 mg/L) due to the generation of 1O2, Fe(IV)=O and •OH. The introduction of sulfur was found to significantly improve the electronic structure and electron transfer efficiency of S–Fe@G. This enhancement promoted the activity of Fe reaction sites and increased the multivalent distribution of Fe. Additionally, sulfur incorporation lowered the reaction energy barrier for PMS dissociation and accelerated the Fe(II)/Fe(III) cycle. These combined effects resulted in the rapid degradation of pollutants and ensured the stable operation of the catalytic system over extended periods. In addition, the nanoconfined space composed of the two-dimensional carbonaceous structure was conducive to the accumulation of pollutants and the rapid activation of PMS. The 2S–20Fe@G catalytic membrane achieved a high selective removal of TC (>94.5 %) and substantial mineralization of pollutants (>52.1 %) in both simulated (Humic acid + TC) and real (Lake water + TC) waters, demonstrating its potential for practical applications.
Date Issued
2025-05-01
Date Acceptance
2025-03-16
Citation
Journal of Membrane Science, 2025, 724
ISSN
0376-7388
Publisher
Elsevier BV
Journal / Book Title
Journal of Membrane Science
Volume
724
Copyright Statement
Copyright © 2025 Elsevier B.V. This is the author’s accepted manuscript made available under a CC-BY licence in accordance with Imperial’s Research Publications Open Access policy (www.imperial.ac.uk/oa-policy)
License URL
Publication Status
Published
Article Number
123984
Date Publish Online
2025-03-17