Phosphonates-enhanced production of reactive oxygen species by ferrous ion in the presence of oxygen: Effects and mechanisms
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING(2024)
Abstract
Due to their potential environmental hazards, the ongoing release of phosphonates into natural water bodies has sparked serious worries. Phosphonates are typically found as metal-phosphonate complexes in natural water and their complex with Fe2+ is predominant. In this study, we demonstrated that phosphonates could enhance reactive oxygen species (ROS) production upon complexation with Fe2+ in the presence of O2 (from the air). Using aminotris (methyphosphonic acid) (ATMP) as a model phosphonate, we thoroughly investigated the effects and mechanism of ROS production in the ATMP/Fe2+/O2 system. OH center dot-mediated oxidation was responsible for the transformation of co-existing contaminants. With oxygen (O-) and nitrogen (N-) in ATMP complexed with Fe2+, the redox potential of Fe2+/Fe3+ was significantly reduced, thus promoting OH center dot production. Further experiments identified OH center dot production followed the one-electron transfer pathway (O2 -> O2 center dot- -> H2O2 -> OH center dot). Due to the generation of OH center dot, 61.5% of phenol (10 mg/L) was degraded and a small fraction of ATMP underwent C-P bond cleavage. The phenomenon of ATMP-enhanced ROS production and co-existing pollutants degradation occurred throughout a wide pH spectrum from 3.0 to 10.0. This study not only clarified how ROS were produced in the ATMP/Fe2+/O2 system, but also provided new ideas for understanding the environmental behavior of phosphonates in promoting co-existing pollutants degradation.
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Key words
Phosphonates,Fe2+-ATMP complex,Oxygen activation,ROS production,Enhancing mechanism
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