Removal of sulfamethoxazole, sulfadiazine, and sulfamethazine by UV radiation and HO• and SO4•− radicals using a response surface model and DFT calculations
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In this work, the degradation of sulfamethazine (SMT), sulfadiazine (SMD), and sulfamethoxazole (SMX) by using UV light, UV/H2O2, and UV/S2O8−2 was analyzed. Direct photolysis was studied by varying the lamp power and the solution pH. DFT calculations were carried out to corroborate the efficiency of the degradation as a function of the solution pH. The variation of the apparent rate constant, kap, was determined in the indirect photolysis by employing an experimental Box-Behnken-type response surface design. The results evidenced that SMX can be efficiently degraded by applying UV radiation independent of the operating conditions. Nevertheless, the quantum yields for SMT and SMD were close to zero, indicating a low energy efficiency for their photochemical transformation. The effect of the solution pH showed that the photodegradation of sulfonamides depends both on the amount of radiation absorbed as the electronic density. Calculations based on density functional theory and supported by the quantum theory of atoms in molecules allowed to describe fragmentation patterns in the systems under study, proving the lability of S14-C2, N17-C18, and N22-O22 bonds, for SMT, SMD, and SMX, respectively. From response surface methodology, four statistically reliable equations were obtained to determine the kap value as a function of the system operating conditions. Finally, SO4•− radicals proved to have a higher reactivity to degrade SMT and SMD compared with HO• radicals regardless of the operating conditions of the system. © 2020, Springer-Verlag GmbH Germany, part of Springer Nature.
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Degradation; DFT calculations; Response surface design; Sulfonamides design; energy efficiency; experimental study; fragmentation; pesticide; photodegradation; photolysis; pollutant removal; quantum mechanics; ultraviolet radiation; hydrogen peroxide; sulfadiazine; sulfadimidine; sulfamethoxazole; density functional theory; kinetics; oxidation reduction reaction; photolysis; ultraviolet radiation; water pollutant; Density Functional Theory; Hydrogen Peroxide; Kinetics; Oxidation-Reduction; Photolysis; Sulfadiazine; Sulfamethazine; Sulfamethoxazole; Ultraviolet Rays; Water Pollutants, Chemical
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