科研之友
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摘要
H2O2- and PDS-based reactions are two typical advanced oxidation processes (AOPs) with different adaptive pH ranges. However, the underlying mechanisms that caused the distinct applicability of these two AOPs have rarely been explored. Herein, a comparative study of H2O2/PDS-based AOPs employing pyrite as a catalyst to degrade acetaminophen (ACT) was reported. The poor ACT degradation in H2O2/pyrite under alkaline conditions was proven to be caused by a lack of (OH)-O-center dot production instead of by the weaker oxidation property of (OH)-O-center dot. The continuous exposure surface behavior induced by the intense acid-production reaction between PDS and pyrite prevented the coverage of iron-containing compounds on the pyrite surface. Therefore, the adaptive pH range in PDS/pyrite could extend from 4 to 10, in contrast to the narrow effective pH range of 4-6 in H2O2/pyrite. Oxidant consumption indicated that H2O2/pyrite possesses a higher oxidation efficiency than PDS/pyrite. The homogenous catalytic effect was non-negligible in PDS/pyrite, whereas heterogeneous catalytic oxidation dominated H2O2/pyrite under acidic conditions. The quenching experiment and electron spin resonance (ESR) spectroscopy demonstrated that the dominant radical species in H2O2/PDS-based AOPs via pyrite at a pH of 4 were (OH)-O-center dot and (OH)-O-center dot/SO4 center dot-, respectively, thus causing different degradation pathways of ACT. In addition, a higher proportion of S consumption was found in H2O2/pyrite, indicating that sulfur also plays a role during the catalytic reaction. The distinct surface reactions between pyrite and H2O2/PDS led to different water treatment applications.
