Engineering the low-coordinated single cobalt atom to boost persulfate activation for enhanced organic pollutant oxidation

Two atomically dispersed cobalt catalysts with different nitrogen coordination numbers (denoted as CoSA-Nx-C) were synthesized and firstly compared to activate peroxydisulfate (PDS) for bisphenol A (BPA) degradation. Theoretical calculations unveiled that lowering the CoN coordination number from fo...

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Bibliographic Details
Published in:Applied catalysis. B, Environmental Environmental, 2022-04, Vol.303, p.120877, Article 120877
Main Authors: Liang, Xiaoying, Wang, Di, Zhao, Zhiyu, Li, Tong, Chen, Zhenhuan, Gao, Yaowen, Hu, Chun
Format: Article
Language:English
Subjects:
Active radicals
Biodegradation
Bisphenol A
Catalysts
Cobalt
Coordination number
Coordination numbers
Durability
Electron density
Electron paramagnetic resonance
Electron spin resonance
Nitrogen
Oxidation
Persulfate conversion
Pollutants
Single-atom catalysts
Wastewater
Wastewater treatment
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Summary:Two atomically dispersed cobalt catalysts with different nitrogen coordination numbers (denoted as CoSA-Nx-C) were synthesized and firstly compared to activate peroxydisulfate (PDS) for bisphenol A (BPA) degradation. Theoretical calculations unveiled that lowering the CoN coordination number from four to three can apparently increase the electron density of the single Co atom in CoSA-N3-C to enhance PDS conversion. The low-coordinated CoSA-N3-C with CoN3 coordination structure displays a high specific activity of 0.067 L min1 m2, which is 1.31 times greater than that of CoSA-N4-C with normal CoN4 configuration (0.051 L min1 m2) in PDS activation. Electron paramagnetic resonance (EPR) measurements and quenching tests confirmed the primary role of sulfate radical (SO4•−) in BPA oxidation over CoSA-N3-C with PDS. Moreover, CoSA-N3-C delivers favorable durability for PDS activation and potential practicability for realistic wastewater remediation. These findings provide a novel and useful avenue to coordination number modulation of SACs for wider environmental applications. [Display omitted] •Single-atom Co catalyst was firstly applied in peroxydisulfate (PDS) activation.•Lowering coordination number can enhance the electron density of single Co atom.•Single-atomic CoN3 sites deliver higher affinity to PDS than CoN4 centers.•Low-coordinated CoSA-N3-C outperforms CoSA-N4-C with CoN4 sites in PDS conversion.•CoSA-N3-C shows good stability and applicability in actual wastewater remediation.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2021.120877