Issue 7, 2024

Highly coordinated Fe–N5 sites effectively promoted peroxymonosulfate activation for degradation of 4-chlorophenol

Abstract

M–Nx single-atom catalysts (SACs) with a high coordination number (x > 4) are effective catalysts for eliminating organic pollutants, while the origin of SACs with high activity still remains elusive. In this work, we successfully synthesized an Fe–N5 SAC with axial N coordination, which exhibited exceptional catalytic performance by peroxymonosulfate (PMS) activation for degrading 4-chlorophenol (4-CP) in a wide pH range (4.0–10.0). The rate constant of Fe–N5 (2.99 min−1) was 6.36 times higher than that of Fe–N4, and the turnover frequency (TOF) of Fe–N5 was found to be 4–149 times higher than those of state-of-the-art SACs and nanocatalysts reported in the literature for 4-CP degradation by PMS activation. Moreover, Fe–N5 was not significantly affected by coexisting substances (HA, HCO3, SO42−, H2PO4, NO3, and Cl) and had satisfactory degradation efficiency for various chlorophenols. Electron paramagnetic resonance (EPR), quenching experiments, and radical probe experiments demonstrated that 1O2 played a key role in the Fe–N5/PMS system for 4-CP degradation. Density functional theory calculations confirmed that a narrower gap between the Fe-3d band center and Fermi level enhanced the electron transfer in Fe–N5, which resulted in promoted PMS activation. In addition, the Fe–N5/PMS system showed good potential for application in real wastewater. The above findings offer important implications for the future of coordination chemistry in designing M–Nx–C SACs (x > 4), highlighting their practical applications in environmental remediation.

Graphical abstract: Highly coordinated Fe–N5 sites effectively promoted peroxymonosulfate activation for degradation of 4-chlorophenol

Supplementary files

Article information

Article type
Paper
Submitted
07 Mar 2024
Accepted
21 May 2024
First published
21 May 2024

Environ. Sci.: Nano, 2024,11, 3092-3103

Highly coordinated Fe–N5 sites effectively promoted peroxymonosulfate activation for degradation of 4-chlorophenol

M. K. Panjwani, F. Gao, T. He, P. Gao, F. Xiao and S. Yang, Environ. Sci.: Nano, 2024, 11, 3092 DOI: 10.1039/D4EN00189C

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