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One-pot preparation of surface vulcanization Co-Fe bimetallic aerogel for efficient sulfadiazine degradation

CHEMICAL ENGINEERING JOURNAL(2022)

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摘要
A novel magnetic surface vulcanized cobalt-iron aerogel (CoFe-S MA) with a self-supporting, crosslinked bimetallic nanowire structure was fabricated via NaBH4-mediated gelation followed by in-situ vulcanization with Na2S solution, which showed efficient sulfadiazine (SDZ) degradation through peroxodisulfate (PDS) activation. The optimized CoFe-0.2S aerogels exhibited the best degradation performance (99.8%) for SDZ (10 mg/L, 100 mL) within 15 min, and the total organic carbon (TOC) removal efficiency reached 53%. The excellent degradation performance was attributed to the accelerated redox process and rapid formation of sulfate radical (SO4-) caused by bimetal synergistic effect, as well as the sufficient exposed active sites provided by the self-supporting hierarchical porous structure of the aerogel. Compared with CoFe-MAs, electrochemical impedance spectroscopy (EIS) demonstrated lower resistance and more rapid charge transfer of CoFe-S MAs, which was ascribed to the presence of delocalized electrons in iron sulfides layer. A high turnover frequency (TOF) of 4.0 L.min(-1).g(-1) was achieved due to that the reduction effect of S-2 on the surface promoted the regeneration of Fe and Co active species. Electron paramagnetic resonance (EPR) and quenching experiments revealed the dominant reactive oxide species (ROS) to be SO4-, center dot OH, and Fe (IV). This work paves the way for the application of metal aerogels in the field of advanced oxidation process based on sulfate radical (AR-AOPs).
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关键词
Transition metal,Aerogels,Advanced oxidation,Peroxodisulfate
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