Peroxymonosulfate oxidation via paralleled nonradical pathways over iron and nitrogen doped porous carbons

被引：28
作者：
Wang, Jun [1 ]
Zhao, Ying [1 ]
Li, Chunting [1 ]
Yu, Zijun [1 ,2 ]
Zhang, Yang [1 ]
Li, Yuan [1 ,2 ]
Tan, Xiaoyao [1 ,2 ]
Liu, Shaomin [3 ]
Wang, Shaobin [4 ]
Duan, Xiaoguang [4 ]
机构：
[1] Tiangong Univ, Sch Environm Sci & Engn, State Key Lab Separat Membranes & Membrane Proc, Tianjin 300387, Peoples R China
[2] Tiangong Univ, Dept Chem Engn, Tianjin 300387, Peoples R China
[3] Beijing Univ Chem Technol, Coll Chem Engn, Beijing 100029, Peoples R China
[4] Univ Adelaide, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia
来源：
SCIENCE OF THE TOTAL ENVIRONMENT | 2022年 / 836卷
基金：
中国国家自然科学基金; 澳大利亚研究理事会; 中国博士后科学基金;
关键词：
Porous carbon; Peroxymonosulfate; High-valent iron-oxo species; Nonradical pathway; Electron-transfer process; PERSULFATE ACTIVATION; DEGRADATION; NANOTUBES; GRAPHENE; SULFAMETHOXAZOLE; CONTAMINANTS;
D O I：
10.1016/j.scitotenv.2022.155670
中图分类号：
X [环境科学、安全科学];
学科分类号：
08 ; 0830 ;
摘要：
Hierarchically porous iron/nitrogen-doped carbons (Fe-N-PC) were developed for the oxidation of ibuprofen (IBP) with peroxymonosulfate (PMS). The incorporation of trace-level iron and nitrogen dopants promoted the catalytic performance remarkably, leading to 4.8, 16.4 and 22.9-fold enhancement over N-doped carbon (N-PC), porous carbon (PC), and Fe-doped carbon (Fe-PC), respectively. Fe(III) was anchored in nitrogen-coordinated pots (Fe-Nx) in the sp2-hybridized carbon network, and graphitic-N could synergistically boost the catalysis. Notably, methyl phenyl sulfoxide (PMSO) transformation, quenching tests, in situ electrochemical analysis and Raman spectroscopy verified highvalent iron-oxo species and direct electron transfer pathway accounted for pollutant oxidation. The relationship between the kinetic constants (lnkobs) and the oxidation peak potential (Eop) of pollutants was established with good correlation, manifesting particular selectivity toward oxidizing electron-rich pollutants and great immunity to background inorganic ions and natural organic matters (NOMs) for real wastewater treatment. The deactivation mechanisms of Fe-N-PC were revealed via surface oxidation and dopant refabrication. This work delicates to deepen the understanding of the nonradical mechanisms and structure-oriented PMS activation by engineered carbonaceous materials.
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页数：11
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