4.7 Article

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

期刊

CHEMICAL ENGINEERING JOURNAL
卷 378, 期 -, 页码 -

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.122071

关键词

Perfluorooctanoic acid; Electro-Fenton; Anodic oxidation; Fe-Mn doped carbon aerogel; Oxygen reduction reaction

资金

  1. National Natural Science Foundation P.R. China [21677106, 21537003]
  2. Science & Technology Commission of Shanghai Municipality [14DZ2261100]
  3. Fundamental Research Funds for the Central Universities
  4. Institute of Water Environmental Engineering Jiangsu Industrial Technology Research Institute (Yancheng) [NDYCKF201710]

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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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