Journal
CHEMICAL ENGINEERING JOURNAL
Volume 384, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.123324
Keywords
Heterogeneous E-Fenton; Triclosan; Oxygen reduction reaction; MOF-derived catalyst; Synergistic activation
Categories
Funding
- National Nature Science Foundation of China [41977316, 21677052]
- Guangdong Water Conservancy Science and Technology Innovation Project (2017-25)
- Guangdong technological innovation strategy of special funds (key areas of research and development program) [2018B020205003]
- Chinese Central Government for Basic Scientific Research Operations in Commonweal Research Institutes [PM-zx703-201602-044]
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Mn/Fe@porous carbon (PC) was successfully fabricated through a simple carbonization of Mn-doped MIL-53(Fe) precursor and used as cathode modification in hydroxyl radical (center dot OH) based heterogeneous electro-Fenton (hetero-EF) process for triclosan (TCS) degradation. With co-doping of bimetal (Mn and Fe) in porous carbon, Mn/Fe@PC could markedly enhance the electrocatalysis with low oxygen reduction potential, high electrochemical active area and low resistance. Mn/Fe@PC modified cathode showed high electrocatalytic activity, great stability and low energy consumption (1.92 kWh m(-1) and 0.63 kWh log(-1) m(-3)) for TCS degradation over a wide pH range. The complete TCS degradation within 120 min and a 56.9 +/- 2.0% TOC removal within 240 min were achieved under the condition of current 40 mA and initial pH 3. Based on the CV curves, the more negative reductive peak of Fe and Mn revealed the kinetically beneficial regeneration of Fe-II/Mn-II/III in Mn/Fe@ PC. The electron transfer between FeII/III and Mn-II/III/IV together with the direct regeneration of Fe-II/ Mn-II/III on the cathode, could markedly promote the utilization of H2O2 eventually leading to facilitating TCS degradation. According to the GC-MS intermediates, the possible TCS degradation pathway was deduced, including hydroxylation and dehalogenation attacked by center dot OH. Furthermore, the TCS degradation experiments were also performed in different water matrix including river water, tap water and municipal sewage, indicating the feasibility of the TCS degradation in actual waters with Mn/Fe@PC-CP cathode in hetero-EF process. The toxicity analysis indicated that the hetero-EF process could achieve the TCS degradation and toxicity reducing.
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