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Nitrogen-Doped Carbon Materials for Persulfate Activation via Electron Transfer Pathways.

Authors :
Jiang Z
Shi Z
Li C
Wang H
Huang Y
Ye L
Source :
Langmuir : the ACS journal of surfaces and colloids [Langmuir] 2024 Oct 01; Vol. 40 (39), pp. 20584-20595. Date of Electronic Publication: 2024 Sep 19.
Publication Year :
2024

Abstract

The incorporation of nitrogen into carbon materials is a strategy that effectively boosts their catalytic potency. Herein, a nitrogen-enriched carbon substance, designated as CN <subscript>0.6</subscript> , was synthesized from melamine, serving as a precursor. This substance has been established to act as an efficient catalyst devoid of metals for the activation of peroxymonosulfate (PMS). At a temperature of 25 °C, a concentration of 0.05 g/L CN <subscript>0.6</subscript> along with 1 mM PMS suffices to achieve the complete degradation of concentrated tetracycline hydrochloride (TC) in a short period of 4 min. This enhanced catalytic performance is attributed to the optimal level of nitrogen doping, which elevates the pyrrolic nitrogen content and introduces additional defects characterized by an I <subscript>D</subscript> / I <subscript>G</subscript> ratio of 1.02. These factors collectively augment the adsorptive capacity for PMS and create a greater number of active sites to facilitate its activation. The dominance of a nonradical electron transfer mechanism in the CN <subscript>0.6</subscript> /PMS system has been confirmed through a series of analyses, including radical identification, quenching tests, and electrochemical assessments. Employing high-resolution liquid chromatography coupled with tandem mass spectrometry (LC-MS), the investigation identified three potential degradation routes for TC. Furthermore, the intermediates produced are determined to possess reduced toxicity in comparison to TC. The findings of this study offer a approach to the synthesis of highly efficient nitrogen-doped, metal-free catalysts, presenting a promising strategy for the degradation of environmental pollutants.

Details

Language :
English
ISSN :
1520-5827
Volume :
40
Issue :
39
Database :
MEDLINE
Journal :
Langmuir : the ACS journal of surfaces and colloids
Publication Type :
Academic Journal
Accession number :
39297556
Full Text :
https://doi.org/10.1021/acs.langmuir.4c02321