Journal
CHEMICAL ENGINEERING JOURNAL
Volume 439, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.135784
Keywords
Persulfate activation; Nitrogen doping; Carboxymethyl chitosan; SMX degradation
Categories
Funding
- National Natural Science Foundation of China [52070121, U1906221]
- Major Program of Shandong Province Technological Innovation Project [2020CXGC011403]
- Guangdong Basic and Applied Basic Research Foundation [2020A1515011400]
- Shenzhen Fundamental Research Program [JCYJ20190807094003691]
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An environmentally friendly Fe@nitrogen-doped carbon nanocomposite catalyst (Fe@N-CNs) was prepared using carboxymethyl chitosan hydrogel as a template. The catalyst showed excellent catalytic activity for the degradation of sulfamethoxazole (SMX) and exhibited stable performance over a wide pH range and under high-salinity conditions. Singlet oxygen was identified as the dominant reactive species in the catalytic oxidation process. The Fe@N-CNs/PMS system also proved to be effective against antibiotic resistant bacteria and antibiotics resistance genes.
An environmentally friendly Fe@nitrogen-doped carbon nanocomposite catalyst (Fe@N-CNs) was prepared via a facile and economical process using carboxymethyl chitosan (CMCs) hydrogel as a template to achieve Fe anchoring and N-doping simultaneously for peroxymonosulfate (PMS) activation to efficiently degrade sulfamethoxazole (SMX). The core-shell structure of Fe@N-CNs displayed that Fe nanoparticles identified as Fe3C and Fe3N were encapsulated in nitrogen-doped carbon nanosheets. The formation of FexNy sites and the high content of graphitic N obtained from CMCs facilitated the catalytic reaction. With excellent catalytic activity to achieve complete degradation of SMX in less than 10 min, Fe@N-CNs/PMS system also exhibited stable catalytic degradation efficiency over a wide pH range (3.0-9.0) and under high-salinity conditions. Singlet oxygen was identified as the dominant reactive species in catalytic oxidation and played a vital role in the non-radical pathway. The potential SMX degradation pathway and mechanism in the Fe@N-CNs/PMS reaction system were proposed according to DFT calculations and product detection results. Quantitative structure-activity relationship (QSAR) prediction verified the efficient elimination of SMX degradation products toxicity. Moreover, the Fe@N-CNs/PMS system was also confirmed to be effective towards the inactivation of antibiotic resistant bacteria (ARB) and antibiotics resistance genes (ARGs).
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