Issue 7, 2022

Efficient activation of peroxymonosulfate by C3N5 doped with cobalt for organic contaminant degradation

Abstract

The activation of peroxymonosulfate (PMS) by metal-doped C–N-based materials has been used extensively for pollutant degradation but usually suffers from low efficiency and stability due to the relatively few N coordination sites, particularly for the degradation of persistent organic pollutants (POPs). To overcome these issues, we have developed a novel N site-abundant C3N5 doped with cobalt for PMS activation to degrade a typical POP (2,4,4′-trichlorobiphenyl, PCB28). It was found that cobalt-doped C3N5 (Co-C3N5) exhibited high activity towards activating PMS for the complete degradation of PCB28 within 30 min (kobs = 0.1998 min−1), which was 11.8–27.8 times higher than that with conventional metal-based persulfate activation processes. X-ray absorption fine structure (XAFS) spectroscopy, electron paramagnetic resonance (EPR), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), density functional theory (DFT) calculations, and radical quenching experiments were combined to clarify the activation mechanism of PMS by Co-C3N5. It was unveiled that isolated single Co atoms coordinated by pyridinic N (Co–N4) were the main active sites for the catalytic decomposition of PMS to produce sulfate radicals for contaminant degradation. In addition, Co-C3N5 has stable catalytic performance with limited Co dissolution within five cycles over a wide range of pH values. This study provides a novel strategy to design highly effective metal-doped C–N-based catalysts for PMS-based advanced oxidation technologies for environmental remediation.

Graphical abstract: Efficient activation of peroxymonosulfate by C3N5 doped with cobalt for organic contaminant degradation

Supplementary files

Article information

Article type
Paper
Submitted
09 mar 2022
Accepted
29 maj 2022
First published
02 jun 2022

Environ. Sci.: Nano, 2022,9, 2534-2547

Efficient activation of peroxymonosulfate by C3N5 doped with cobalt for organic contaminant degradation

T. Li, P. Cui, X. Wang, C. Liu, Y. Zeng, G. Fang, Y. Zhao, J. Gao, Y. Wang and D. Zhou, Environ. Sci.: Nano, 2022, 9, 2534 DOI: 10.1039/D2EN00216G

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