Nitrogen-doped carbon nanosheets with Fe-based nanoparticles for highly efficient degradation of antibiotics and sulfate ion enhancement effect

Wenkai Song; Zenglong Wu; Xiangwei Xu; Haijie Wu; Yuyuan Yao

doi:10.1016/j.chemosphere.2022.133704

Nitrogen-doped carbon nanosheets with Fe-based nanoparticles for highly efficient degradation of antibiotics and sulfate ion enhancement effect

Chemosphere. 2022 May:294:133704. doi: 10.1016/j.chemosphere.2022.133704. Epub 2022 Jan 20.

Authors

Wenkai Song¹, Zenglong Wu¹, Xiangwei Xu¹, Haijie Wu¹, Yuyuan Yao²

Affiliations

¹ National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Hangzhou, 310018, PR China.
² National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Hangzhou, 310018, PR China. Electronic address: yyy0571@126.com.

PMID: 35066083
DOI: 10.1016/j.chemosphere.2022.133704

Abstract

Developing Fe-based catalysts with high-effective and environmentally friendly features in Fenton-like system for treating wastewater is still a challenge. Novel nitrogen-doped carbon nanosheets with Fe⁰/Fe₃C nano-particles (Fe@NCS-900) were prepared through a simple solvent-free strategy by pyrolyzing the mixture of 2,6-diaminopyridine and ferric chloride hexahydrate under 900 °C. The Fe@NCS-900 possessed almost 100% removal efficiency and 66.5% mineralization rate for the degradation of CBZ in 10 min. Moreover, the Fe@NCS-900 exhibited an apparent first-order constant as high as 0.8809 min^-1, which is 22 and 29 times higher than that of the commercial Fe⁰ and traditional Fenton system, respectively, which could be attribute to the high graphitization degree and rich nitrogen content. Besides, the results of the radical quenching experiments, electron paramagnetic resonance (EPR) and the probe experiments demonstrated that a large number of high valent iron species (Fe (IV)) besides singlet oxygen (¹O₂) and superoxide radicals (O₂^•-) existed and contributed to the CBZ degradation. More interestingly, the addition of coexisting anion SO₄^2- in the reaction system could significantly boost the concentration of •OH and SO₄^•- by 28.3 times and 9.7 times, respectively, resulting in the increase of the apparent first-order constant by 5.9 times (5.1733 min^-1), which was entirely different from previous reports that SO₄^2- had no effect on the catalytic activity or even displayed slightly inhibitory effect. In addition, the catalyst exhibited broad pH adaptability in the pH range of 2-9. The intermediate products of CBZ degradation were investigated by liquid chromatography mass spectrometry (LC-MS) and the degradation pathway was proposed. This paper provides new insights for developing a promising Fe-based nitrogen-doped catalyst for practical wastewater treatment.

Keywords: Fe(0)/Fe(3)C nano-particles; Organics degradation; PMS activation; Sulfate ion enhancement effect.

MeSH terms

Anti-Bacterial Agents
Carbon*
Nanoparticles*
Nitrogen
Peroxides / chemistry
Sulfates

Substances

Anti-Bacterial Agents
Peroxides
Sulfates
Carbon
Nitrogen