Light and nitrogen vacancy-intensified nonradical oxidation of organic contaminant with Mn (III) doped carbon nitride in peroxymonosulfate activation

Qishi Si; Huazhe Wang; Junyan Kuang; Banghai Liu; Shanshan Zheng; Qi Zhao; Wenrui Jia; Yaohua Wu; Hao Lu; Qinglian Wu; Tao Yu; Wanqian Guo

doi:10.1016/j.jhazmat.2023.131463

Light and nitrogen vacancy-intensified nonradical oxidation of organic contaminant with Mn (III) doped carbon nitride in peroxymonosulfate activation

J Hazard Mater. 2023 Jul 15:454:131463. doi: 10.1016/j.jhazmat.2023.131463. Epub 2023 Apr 21.

Authors

Qishi Si¹, Huazhe Wang¹, Junyan Kuang¹, Banghai Liu¹, Shanshan Zheng¹, Qi Zhao¹, Wenrui Jia¹, Yaohua Wu¹, Hao Lu¹, Qinglian Wu¹, Tao Yu², Wanqian Guo³

Affiliations

¹ State Key Laboratory of Urban Water Resource and Environment, Harbin Inst Technology, Harbin, Heilongjiang 150090 People's Republic of China.
² Tianjin Univ, Sch Chem Eng & Technol, Tianjin 300350, People's Republic of China.
³ State Key Laboratory of Urban Water Resource and Environment, Harbin Inst Technology, Harbin, Heilongjiang 150090 People's Republic of China. Electronic address: guowanqian@hit.edu.cn.

PMID: 37141778
DOI: 10.1016/j.jhazmat.2023.131463

Abstract

Recently, Mn-based materials have a great potential for selective removal of organic contaminants with the assistance of oxidants (PMS, H₂O₂) and the direct oxidation. However, the rapid oxidation of organic pollutants by Mn-based materials in PMS activation still presents a challenge due to the lower conversion of surface Mn (III)/Mn (IV) and higher reactive energy barrier for reactive intermediates. Here, we constructed Mn (III) and nitrogen vacancies (Nv) modified graphite carbon nitride (MNCN) to break these aforementioned limitations. Through analysis of in-situ spectra and various experiments, a novel mechanism of light-assistance non-radical reaction is clearly elucidated in MNCN/PMS-Light system. Adequate results indicate that Mn (III) only provide a few electrons to decompose Mn (III)-PMS* complex under light irradiation. Thus, the lacking electrons necessarily are supplied from BPA, resulting in its greater removal, then the decomposition of the Mn (III)-PMS* complex and light synergism form the surface Mn (IV) species. Above Mn-PMS complex and surface Mn (IV) species lead to the BPA oxidation in MNCN/PMS-Light system without the involvement of sulfate (SO₄^{• ̶}) and hydroxyl radicals (•OH). The study provides a new understanding for accelerating non-radical reaction in light/PMS system for the selective removal of contaminant.

Keywords: Light assistance; Mn-PMS complex; Nitrogen vacancy; Non-radical reaction; Surface Mn (IV) species.