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Sulfite activation on a silica-supported well-dispersed cobalt catalyst via an electron transfer complex path
被引:45
作者:
Ding, Wei
[1
]
Xiao, Weilong
[1
]
Huang, Wenxuan
[1
]
Sun, Qiang
[1
]
Zheng, Huaili
[1
]
机构:
[1] Chongqing Univ, Key Lab Three Gorges Reservoir Reg Ecoenvironm, State Minist Educ, Chongqing 400045, Peoples R China
基金:
中国国家自然科学基金;
中国博士后科学基金;
关键词:
Cobalt ammine complex;
Surface complex;
Sulfite activation;
Oxysulfur radicals;
Advanced oxidation process;
ACID ORANGE 7;
ADVANCED OXIDATION;
ORGANIC CONTAMINANTS;
RADICAL GENERATION;
DEGRADATION;
WATER;
REMOVAL;
SYSTEM;
DYE;
AUTOXIDATION;
D O I:
10.1016/j.jclepro.2020.120457
中图分类号:
X [环境科学、安全科学];
学科分类号:
08 ;
0830 ;
摘要:
The metal activating sulfite system has attracted widespread attention as a novel advanced oxidation process recently. In this study, a silica-supported highly dispersed cobalt catalyst was prepared using Co ammine complex as precursor, characterized by transmission electron microscope, X-ray diffraction, Brunauer-Emmett-Teller surface area, X-ray photoelectron spectroscopy and so forth, and used to activate sulfite for the removal of organic pollutants. The as-prepared catalyst displayed a durable and remarkable catalytic activation of sulfite for organic degradation in sequential experiments. The mechanistic study corroborated the dual roles of sulfite as a complexing ligand on catalyst surface and a precursor of oxysulfur radicals. The surface-bound and free SO4 center dot- were found to be the dominating radicals responsible for organic degradation. The steady-state approximation of SO4 center dot- were examined and the apparent reaction rate constant of SO4 center dot- generation was 0.60 +/- 0.07 M-1 s(-1) at 0.25 g L-1 catalyst. The influencing factors and operating parameters, including catalyst dosage, sulfite/contaminant ratio, pH, temperature, anions and natural organic matter were investigated and optimized systematically. As conclusion, the as-prepared catalyst to efficient activation of sulfite can be proposed as a promising advanced oxidation process based on oxysulfur radicals for the treatment of wastewater. (C) 2020 Elsevier Ltd. All rights reserved.
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