Efficiently degradation of perfluorooctanoic acid in synergic electrochemical process combining cathodic electro-Fenton and anodic oxidation

被引:91
|
作者
Wang, Qingning [1 ,2 ]
Liu, Mingyue [1 ,2 ]
Zhao, Hongying [1 ,2 ,3 ,4 ]
Chen, Ying [1 ,2 ]
Xiao, Fan [1 ,2 ]
Chu, Wenhai [5 ]
Zhao, Guohua [1 ,2 ]
机构
[1] Tongji Univ, Sch Chem Sci & Engn, Siping Rd 1239, Shanghai 200092, Peoples R China
[2] Tongji Univ, Shanghai Key Lab Chem Assessment & Sustainabil, Siping Rd 1239, Shanghai 200092, Peoples R China
[3] Nanjing Univ, Yancheng 224001, Peoples R China
[4] Yancheng Acad Environm Protect Technol & Engn, Yancheng 224001, Peoples R China
[5] Tongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
关键词
Perfluorooctanoic acid; Electro-Fenton; Anodic oxidation; Fe-Mn doped carbon aerogel; Oxygen reduction reaction; PFOA; MINERALIZATION; SULFONATE; COMPOSITE; REMOVAL; PERFORMANCE; FABRICATION; REDUCTION; MECHANISM; KINETICS;
D O I
10.1016/j.cej.2019.122071
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A synergic electrochemical process between cathodic electro-Fenton and anodic oxidation was proposed for efficient degradation of perfluorooctanoic acid (PFOA) in this work. The electron-transfer ability and hydroxyl radicals (center dot OH) concentration are the key parameters for the PFOA degradation efficiency. Boron-doped diamond (BDD) anode exhibited the highest anodic oxidation ability compared to platinum and carbon stick. The integrated FeMn-doped carbon aerogel was fabricated as cathode for in-situ enhancing the generation of center dot OH. The X-ray photoelectron spectroscopy (XPS) and near-edge X-ray absorption fine structure (NEXAFS) indicated the main composition of cathode is Fe-0 and MnO. The Fe in the integrated cathode favors the electro-catalytic ability of oxygen reduction reaction (ORR), while MnO enhances the selectivity of 2-electron ORR with H2O2 as main product. The electroformed H2O2 would be onsite catalytic decomposition with Fe-II and Mn-II as Fenton catalysts for in-situ generating center dot OH radicals. The optimal cathode with Fe/10Mn weight ratio can generate the highest concentration of center dot OH. The catalytic degradation efficiency in this synergic electro-catalysis process with BDD as anode and Fe10MnC as cathode reached nearly 97% PFOA removal and 93% TOC removal after 4?h, suggesting the prominent synergic combination of cathodic electro-Fenton and anodic oxidation. The amount of intermediates C6F13COO- was decreased while others including C5F11COO-, C4F9COO-, C3F7COO-, C2F5COO-, CF3COO- were increased with increasing electro-catalysis time. The NEXAFS analysis of F in solution and cathode surface further confirmed the continuously synergic electro-catalysis between anodic and cathodic electro-Fenton oxidation.
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页数:13
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