MgFe2O4/MgO modified biochar with oxygen vacancy and surface hydroxyl groups for enhanced peroxymonosulfate activation to remove sulfamethoxazole through singlet oxygen-dominated nonradical oxidation process

被引:35
作者
Sun, Zhenhua [1 ]
Li, Jing [2 ,3 ]
Wang, Xuejiang [1 ]
Zhang, Yanan [4 ]
Xia, Siqing [1 ]
机构
[1] Tongji Univ, Shanghai Inst Pollut Control & Ecol Secur, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resource Reuse, Shanghai 200092, Peoples R China
[2] Shanghai Invest Design & Res Inst Co Ltd, Shanghai 200050, Peoples R China
[3] China Three Gorges Corp, YANGTZE Eco Environm Engn Res Ctr, Beijing 100038, Peoples R China
[4] Tongji Univ, Sch Chem Sci & Engn, Shanghai 200092, Peoples R China
基金
中国博士后科学基金;
关键词
Peroxymonosulfate activation; Singlet oxygen; Oxygen vacancy; Surface-OH groups; PERSULFATE ACTIVATION; DEGRADATION; GENERATION; RADICALS; SULFATE; WATER;
D O I
10.1016/j.cej.2023.146960
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Nonradical oxidation plays a crucial role in the contaminant degradation due to their high selectivity and anti-interference ability. In this study, we report that peroxymonosulfate (PMS) activated by MgFe2O4/MgO modified biochar (MMFBC) achieves almost complete nonradical oxidation process dominated by 1O2 for degradation of sulfamethoxazole (SMX). The experimental results show that MMFBC exhibits excellent performance for SMX degradation, and is not susceptible to interference from coexisting ions and different water matrices. Oxygen vacancy (OV) and surface -OH groups on MMFBC surface are detected and considered to be crucial for non-radical processes. Characterizations and theoretical calculations reveal that the co-adsorbed PMS and dissolved oxygen (O2) near OV form a localized high-density electron transfer process. With the premise of hydrogen bonding between PMS and surface -OH groups, PMS acts as an electron donor to OV, which in turn transfers electron to O2 through the iron cycle involving Fe(II)/Fe(III). Finally, the electron acceptor O2 undergoes con-version into center dot O2-, which subsequently transforms into 1O2 to achieve nonradical oxidation processes. This work provides an in-depth investigation into the OV and surface -OH groups mediated nonradical oxidation mech-anism, and proposes a novel insight into electron-transfer processes among PMS, O2 and catalyst.
引用
收藏
页数:11
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