Exploring degradation properties and mechanisms of emerging contaminants via enhanced directional electron transfer by polarized electric fields regulation in Fe-N4-Cx

被引:12
|
作者
Wang, Yan [1 ]
Xiao, Tong [1 ]
Zuo, Shiyu [1 ]
Wan, Jinquan [1 ,2 ]
Yan, Zhicheng [1 ]
Zhu, Bin [3 ]
Zhang, XiaoLong [4 ]
机构
[1] South China Univ Technol, Sch Environm & Energy, Guangzhou, Peoples R China
[2] Guangdong Plant Fiber High Valued Cleaning Utiliza, Guangzhou, Peoples R China
[3] Guangdong Zihua Technol Co Ltd, Foshan, Peoples R China
[4] Univ Sci & Technol China, Div Nanomat & Chem, Hefei Natl Lab Phys Sci Microscale, Hefei, Peoples R China
基金
中国国家自然科学基金;
关键词
Polarized electric field; Emerging contaminants; Electron -directed transport; Defects; METAL-ORGANIC FRAMEWORK; POROUS CARBON; OXIDATION; PEROXYMONOSULFATE; ACTIVATION; CATALYST; SULFAMETHOXAZOLE; ENVIRONMENT; KINETICS; REMOVAL;
D O I
10.1016/j.jhazmat.2022.130698
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Heterogeneous catalysis offers an opportunity to overcome the low efficiency and secondary pollution limitations of emerging contaminants (ECs) purification technologies, but it is still challenging to regulate electron directed transport for achieving high catalysis efficiency and selectivity due to insufficient understanding of the electron transfer pathways and behavioral mechanisms during its catalysis. Here, by tuning the defects of the C-N co-ordination of the support, the polarized electric field (PEF) characteristics are changed, which in turn affects the electron transport behavior. The results show that the charge offset on Fe-N4-Cx forms a PEF, which will induce directional electron transport. After the quantitative structure-activity relationship (QSAR) fitting analysis, the greater the degree of C-N defects, the higher the intensity of the PEF, which in turn enhances the electron transport and promotes the catalytic behavior. In addition, the surface pyrrole N site can adsorb enrofloxacin (ENR) and enrich it on the surface. This can reduce the transport distance of reactive oxygen species (ROS) to synergize catalysis and adsorption, resulting in rapid degradation of ECs. Combined with liquid chromatograph mass spectrometer (LC-MS) results and theoretical calculations, five degradation pathways of ENR were spec-ulated, mainly including the oxidation of piperazine and the cleavage of the quinolone ring. This work proposes a novel PEF regulation strategy and explores its mechanism for safe treatment of ECs.
引用
收藏
页数:13
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