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Mechanistic investigation in degradation mechanism of 5-Fluorouracil using graphitic carbon nitride

[Display omitted] •Investigation in degradation mechanism of pharmaceutical drug 5-Fluorouracil.•Synthesis of highly stable g-C3N4 using ultrasound-assisted pyrolytic technique.•Highly photo-active g-C3N4 with same catalytic activity after 5 runs of experiments.•Positive synergy effect with a factor...

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Published in:Ultrasonics sonochemistry 2019-01, Vol.50, p.311-321
Main Authors: Dinesh, G. Kumaravel, Chakma, Sankar
Format: Article
Language:English
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Summary:[Display omitted] •Investigation in degradation mechanism of pharmaceutical drug 5-Fluorouracil.•Synthesis of highly stable g-C3N4 using ultrasound-assisted pyrolytic technique.•Highly photo-active g-C3N4 with same catalytic activity after 5 runs of experiments.•Positive synergy effect with a factor of 2.4 in sono-hybrid Advanced Oxidation Processes. The present study reports the synthesis of metal-free polymeric catalyst, graphitic carbon nitride (g-C3N4), through sonochemical method followed by thermal treatment. The synthesized g-C3N4 was characterized using XRD, DRS, FESEM, TGA, EDX, etc. and the characterization results revealed that it possesses medium band-gap energy, high thermal and chemical stability. The photo-activity of the catalyst was also evaluated using degradation of 5-Fluorouracil under different experimental conditions. The results revealed that the addition of H2O2 during sonolysis process did not show any significant synergy. This is attributed to the low vapor pressure of H2O2 that does not allow it to diffuse into the cavitation bubble to produce OH radicals through sonolysis process. Using sono-hybrid process, more than 90% degradation was seen within 5 min of treatment with a rate constant of 3.95 × 10−2 s−1. In alkaline medium, 5-Fluorouracil degradation occurred through defluorination and subsequently substitution of –OH group to the aromatic ring leading to formation of intermediates such as 2-fluoro-3-oxopropanoic acid and urea. While sono-hybrid advanced oxidation processes (AOPs) helped towards complete mineralization through formation of smaller molecular compounds such as maleic acids, lactic acids, propanol, etc. On the other hand, the maximum synergy effect of ∼2.4 was seen for sonocatalysis process followed by hybrid-AOPs of (US + g-C3N4 + H2O2 + UVC) with a synergy factor of ∼2.2. Also, the synthesized catalyst exhibited the same catalytic activity even after 5 runs of sono-photocatalysis process for degradation of 5-Fluorouracil.
ISSN:1350-4177
1873-2828
DOI:10.1016/j.ultsonch.2018.09.032