Selective degradation of organic micropollutants by activation of peroxymonosulfate by Se@NC: Role of Se doping and nonradical pathway mechanism

Yandong Chai; Hongling Dai; Peng Zhan; Zhaochen Liu; Zhen Huang; Chaoqun Tan; Fengping Hu; Xing Xu; Xiaoming Peng

doi:10.1016/j.jhazmat.2023.131202

Selective degradation of organic micropollutants by activation of peroxymonosulfate by Se@NC: Role of Se doping and nonradical pathway mechanism

J Hazard Mater. 2023 Jun 15:452:131202. doi: 10.1016/j.jhazmat.2023.131202. Epub 2023 Mar 15.

Authors

Yandong Chai¹, Hongling Dai¹, Peng Zhan², Zhaochen Liu¹, Zhen Huang¹, Chaoqun Tan³, Fengping Hu¹, Xing Xu⁴, Xiaoming Peng⁵

Affiliations

¹ School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China.
² Jiangxi Water Resources Institute, Nanchang 330013, PR China.
³ Department of Municipal Engineering, Southeast University, Nanjing 210000, PR China.
⁴ Shandong Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Shandong University, Qingdao 266237, PR China.
⁵ School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, PR China. Electronic address: pengxiaoming70@ecjtu.edu.cn.

PMID: 36934627
DOI: 10.1016/j.jhazmat.2023.131202

Abstract

In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/PMS* could oxidize phenol by the rapid decomposition of PMS. Specifically, electrons are extracted by Se@NC-900/PMS* and then transferred to the surface of Se@NC-900, which can trigger the degradation of phenol. Notably, it is found that the local charge redistribution caused by the doping of Se can activate the catalytic potential of the intrinsically inert carbon skeleton through density flooding theory (DFT) calculations. The XLogP, ΔE, VIP, and E_{LUMO (Se@NC/PMS)-HOMO (pollutants)} and degradation rate constants of different micropollutants were correlated well linearly. This indicates that the Se@NC-900/PMS system has a great selectivity for the degradation of pollutants. Overall, these findings not only illustrate the role of Se in tuning the electronic structure of Se@NC-x to enhance the activation of PMS, but also bridge the gap in our knowledge about the physicochemical properties and degradation performance of Se@NC catalysts.

Keywords: Degradation performance; Electronic structure; Open-circuit potential; Se.