How metal/support interaction improved degradation performance in the peroxymonosulfate activation process: significance of high-valent cobalt-oxo species

Abstract

Currently, the strategy of metal loading is expected to promote the nonradical catalytic activity of transition metal spinel oxide catalysts in peroxymonosulfate (PMS) systems, but the connection between the mechanism of degradation performance improvement and metal–support interaction (MSI) remains unclear. Herein, a novel CoFe2O4 loaded sepiolite composite (10-CFS) was prepared for PMS activation to degrade ciprofloxacin (CIP). 10-CFS exhibited outstanding PMS activation ability, and 98.7% of CIP was degraded within 30 min, which was significantly higher than that of the physical mixture of sepiolite and CoFe2O4 (59.8%). A series of experiments demonstrated that the presence of Co(IV)[double bond, length as m-dash]O caused the better degradation performance of 10-CFS. Notably, theoretical calculations signified that MSI not only promoted the coupled electron–proton transfer (CEPT) process and thus changed the formation pathway of Co(IV)[double bond, length as m-dash]O, but also facilitated PMS adsorption on 10-CFS and lowered the energy barrier for Co(IV)[double bond, length as m-dash]O generation. In summary, this study illustrates deeply the mechanism of catalytic performance improvement after metal loading by focusing on the MSI and bridges the gap in understanding the MSI and degradation performance.

Graphical abstract: How metal/support interaction improved degradation performance in the peroxymonosulfate activation process: significance of high-valent cobalt-oxo species

Supplementary files

Article information

Article type
Paper
Submitted
23 apr 2024
Accepted
10 sep 2024
First published
27 sep 2024

Environ. Sci.: Nano, 2024, Advance Article

How metal/support interaction improved degradation performance in the peroxymonosulfate activation process: significance of high-valent cobalt-oxo species

X. Fan, W. Zhang, H. Yan, C. Lai, D. Ma, S. Liu, M. Zhang, L. Li, X. Zhou, X. Huo, F. Xu, X. Hu, B. Wang, H. Sun and W. He, Environ. Sci.: Nano, 2024, Advance Article , DOI: 10.1039/D4EN00355A

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