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

Journal 2019 · IF 8.355 · 发表于 2019 年 6 月 24 日
作者: Qingning Wang,Mingyue Liu,Hongying Zhao,Ying Chen,Fan Xiao,Wenhai Chu,Guohua Zhao
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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 ( 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 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 H 2 O 2 as main product. The electroformed H 2 O 2 would be onsite catalytic decomposition with Fe II and Mn II as Fenton catalysts for in-situ generating OH radicals. The optimal cathode with Fe/10Mn weight ratio can generate the highest concentration of 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 C 6 F 13 COO − was decreased while others including C 5 F 11 COO − , C 4 F 9 COO − , C 3 F 7 COO − , C 2 F 5 COO − , CF 3 COO − 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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