Highly dispersed Fe7S8 anchored on sp2/sp3 hybridized carbon boosting peroxymonosulfate activation for enhanced EOCs elimination though singlet oxygen-dominated nonradical pathway

Zijian Jiang; Jia Wei; Xiruo Niu; Xueru Cui; Yanan Li; Nan Cui; Jiamei Li; Jiangkai Huo; Linhao Wang; Wei Ji; Jun Li

doi:10.1016/j.jhazmat.2023.132607

Highly dispersed Fe₇S₈ anchored on sp²/sp³ hybridized carbon boosting peroxymonosulfate activation for enhanced EOCs elimination though singlet oxygen-dominated nonradical pathway

J Hazard Mater. 2024 Jan 5:461:132607. doi: 10.1016/j.jhazmat.2023.132607. Epub 2023 Sep 21.

Authors

Zijian Jiang¹, Jia Wei², Xiruo Niu¹, Xueru Cui¹, Yanan Li¹, Nan Cui¹, Jiamei Li¹, Jiangkai Huo¹, Linhao Wang¹, Wei Ji¹, Jun Li¹

Affiliations

¹ College of Architecture Engineering, Beijing University of Technology, 100 Pingleyuan, Chaoyang District, Beijing 100124, China.
² College of Architecture Engineering, Beijing University of Technology, 100 Pingleyuan, Chaoyang District, Beijing 100124, China. Electronic address: weij@bjut.edu.cn.

PMID: 37757558
DOI: 10.1016/j.jhazmat.2023.132607

Abstract

The synergistic effect of carbon materials with high sp²/sp³ hybridized carbon ratio and metal materials can enhance the efficiency of peroxymonosulfate (PMS) based advanced oxidation processes. In this study, a composite of highly dispersed Fe₇S₈ anchored on sp²/sp³ hybridized carbon (Fe₇S₈@HC) was developed by a facile synthesis for PMS activation. Within 10 min, the removal efficiency of the target pollutant doxycycline (DOX) could reach ca. 96 % in optimal Fe₇S₈@HC/PMS system through a ¹O₂-dominated non-radical pathway. Correlation mechanism analysis revealed that thiophene S, sp²/sp³ ratio and Fe(II) were critical factors for elongating of the O-O bond of PMS. Moreover, the Fe₇S₈@HC/PMS system exhibited favorable adaptability to interference such as common inorganic anions, humic acid and pH changes and could effectively remove various organic pollutants with low ionization potential. Moreover, the system maintained high DOX removal efficiency by running 30 cycles in a continuous flow reactor. Finally, susceptible sites of DOX and four degradation pathways were proposed by density functional theory calculation and LC-MS detection. This work not only offered new insights into the design of high-performance catalysts combining metal and biomass-based carbon materials, but also provided technical support for the remediation of water bodies containing emerging organic contaminants.

Keywords: Emerging organic contaminants; Fe(7)S(8); Hybridized carbon; Peroxymonosulfate; Singlet oxygen.