Degradation of sulfamethoxazole by persulfate assisted micrometric Fe0 in aqueous solution
•Sulfamethoxazole is fully degraded in Fe0/PS systems at room temperature.•Very low un-washed iron load can sustain PS activation over 3 cycles of 1h each.•The reaction stoichiometric efficiency reaches 5.2% under controlled conditions.•Sulfate radicals are quenched by an excess of iron particles.•B...
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Veröffentlicht in: | Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2013-07, Vol.228, p.1168-1181 |
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Sprache: | eng |
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Zusammenfassung: | •Sulfamethoxazole is fully degraded in Fe0/PS systems at room temperature.•Very low un-washed iron load can sustain PS activation over 3 cycles of 1h each.•The reaction stoichiometric efficiency reaches 5.2% under controlled conditions.•Sulfate radicals are quenched by an excess of iron particles.•Bicarbonate delays iron corrosion and limits Fe2+ release into the solution.
Persulfate (PS) chemical activation using micrometric Fe0 particles (MIPs) was tested on sulfamethoxazole (SMX) solution (39.5μM). MIPs load (0.89–17.85mM), PS content (0.4–1.0mM), pH (5.50–8.30) and alkalinity (bicarbonate) were investigated for the improvement of SMX degradation. Optimum conditions for the enhancement of the reaction stoichiometric efficiency (RSE=5.2%) were developed. HPLC–MS results confirmed that SMX was converted into its reduced form through cleavage of the isoxazole N–O bond by two routes: (i) electron abstraction upon sulfate radicals (SRs) attack yielding non stable radical cation SMX+ or (ii) electron addition through Fe0 oxidation yielding unstable radical anion SMX−. In both cases, the final transformation product was identified as b-aminoenone after acceptance of electrons originated from the MIPs surface and protons present in the acidic medium. This suggested that PS activated into SRs was responsible of the rapid degradation of SMX and its transformation product as well in contrast to Fe0 alone. Different water matrices were evaluated in order to understand the role that dissolved ions play on the reaction degradation rate. Successive experiments (n=3) of 1h each conducted on remaining Fe0 showed complete SMX degradation. The extent of SMX mineralization under the experimental conditions reached 37% making from Fe0/PS system an excellent source of SRs able to sustain oxidation reactions in aqueous media of slightly acidic pH. |
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ISSN: | 1385-8947 1873-3212 |
DOI: | 10.1016/j.cej.2013.05.045 |