Enhanced electrochemical-activation of H2O2 to produce •OH by regulating the adsorption of H2O2 on nitrogen-doped porous carbon for organic pollutants removal

被引:19
|
作者
Tan, Zijun [1 ]
Qin, Xin [1 ]
Cao, Peike [1 ]
Chen, Shuo [1 ]
Yu, Hongtao [1 ]
Su, Yan [2 ]
Quan, Xie [1 ]
机构
[1] Dalian Univ Technol, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn, Minist Educ, Dalian 116024, Peoples R China
[2] Dalian Univ Technol, Sch Phys, Key Lab Mat Modificat Laser Ion & Electron Beams, Dalian 116024, Peoples R China
基金
中国国家自然科学基金;
关键词
Hydroxyl radicals; Hydrogen peroxide; Electrochemical-reduction; Nitrogen-doping; HETEROGENEOUS ELECTRO-FENTON; ADVANCED OXIDATION PROCESSES; METAL-FREE CATALYSTS; OXYGEN REDUCTION; HYDROGEN-PEROXIDE; WASTE-WATER; IN-SITU; GRAPHENE; DEGRADATION; ELECTROCATALYSTS;
D O I
10.1016/j.jhazmat.2023.131925
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The heterogeneous Fenton oxidation is regarded as a promising technology for refractory organic pollutants removal relying on highly active & BULL;OH generated via the decomposition of H2O2 catalyzed by iron-based catalyst that overcomes the issues of pH limitation and iron sludge discharge encountered in conventional Fenton reaction. However, the efficiency of & BULL;OH production in heterogeneous Fenton remains low as the limited mass transfer between H2O2 and catalysts caused by the poor H2O2 adsorption. Here, a nitrogen-doped porous carbon (NPC) catalyst with tunable N configuration was prepared for electrochemical-activation of H2O2 to & BULL;OH by enhancing the H2O2 adsorption on catalysts. The resultant & BULL;OH production yield on NPC reached 0.83 mM in 120 min. Notably, the NPC catalyst could be more energy-efficient for actual coking wastewater treatment with an energy consumption of 10.3 kWh kgCOD  1 than other electro-Fenton catalysts reported (20-29.7 kWh kgCOD  1 ). Density function theory (DFT) revealed that highly efficient & BULL;OH production was ascribed to the graphitic N which enhances the adsorption energy of H2O2 on NPC catalyst. This study provides new insight into the fabrication of efficient carbonaceous catalysts by rationally modulating electronic structures for refractory organic pollutants degradation.
引用
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页数:10
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