Nitrogen-doping positively whilst sulfur-doping negatively affect the catalytic activity of biochar for the degradation of organic contaminant

被引:333
作者
Ding, Dahu [1 ]
Yang, Shengjiong [2 ]
Qian, Xiaoyong [3 ]
Chen, Liwei [1 ]
Cai, Tianming [1 ]
机构
[1] Nanjing Agr Univ, Coll Resources & Environm Sci, Nanjing 210095, Peoples R China
[2] Xian Univ Architecture & Technol, Sch Environm & Municipal Engn, Xian 710055, Peoples R China
[3] Shanghai Acad Environm Sci, Shanghai 200233, Peoples R China
基金
中国国家自然科学基金;
关键词
Peroxymonosulfate; Singlet oxygen; Non-radical; Catalytic mechanism; Computational analysis; REDUCED GRAPHENE OXIDE; PERSISTENT FREE-RADICALS; DOPED GRAPHENE; OXYGEN-REDUCTION; HETEROGENEOUS CATALYSTS; ADVANCED OXIDATION; CARBON NANOTUBES; FACILE SYNTHESIS; RATE CONSTANTS; POROUS CARBON;
D O I
10.1016/j.apcatb.2019.118348
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Developing low-cost and efficient metal-free carbon-based catalysts is of great importance but remains a challenge. In this work, rice straw derived biochar was prepared and doped with heteroatoms (N and S) for the catalytic degradation of metolachlor (MET) through activating peroxymonosulfate (PMS). Adsorption process played a critical role for the subsequent degradation process. Surface ketone C (-C = O) was the catalytic active sites for the PMS decomposition. Interestingly, N-doping positively whilst S-doping negatively influenced the MET degradation process. Through experimental investigation and theoretical calculations, N-doping was demonstrated to be beneficial for the interaction between biochar and PMS, thus accelerating the catalytic degradation process. The reactive oxidative species involved in the degradation process were explored by EPR analysis. The degradation pathways were elucidated based on the liquid chromatography time-of-flight mass (LC-TOF-MS) analysis of the degradation products. This study highlights the applications of biochar for the environmental catalysis.
引用
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页数:15
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