期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 50, 期 4, 页码 1731-1740出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.5b03939
关键词
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资金
- Sustainable Systems (SS) Scientific Focus Area (SFA) program at LBNL - U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, Subsurface Biogeochemical Research Program [DE-AC02-05CH11231]
Despite the biogeochemical significance of the interactions between natural organic matter (NOM) and iron species, considerable uncertainty still remains as to the exact processes contributing to the rates and extents of complexation and redox reactions between these important and complex environmental components. Investigations on the reactivity of low-molecular-weight quinones, which are believed to be key redox active compounds within NOM, toward iron species, could provide considerable insight into the kinetics and mechanisms of reactions involving NOM and iron. In this study, the oxidation of 2-methoxyhydroquinone (MH(2)Q) by ferric iron (Fe(III)) under dark conditions in the absence and presence of oxygen was investigated within a pH range of 4-6. Although Fe(III) was capable of stoichiometrically oxidizing MH(2)Q under anaerobic conditions, catalytic oxidation of MH(2)Q was observed in the presence of O-2 due to further cycling between oxygen, semiquinone radicals, and iron species. A detailed kinetic model was developed to describe the predominant mechanisms, which indicated that both the undissociated and monodissociated anions of MH(2)Q were kinetically active species toward Fe(III) reduction, with the monodissociated anion being the key species accounting for the pH dependence of the oxidation. The generated radical intermediates, namely semiquinone and superoxide, are of great importance in reaction-chain propagation. The kinetic model may provide critical insight into the underlying mechanisms of the thermodynamic and kinetic characteristics of metal organic interactions and assist in understanding and predicting the factors controlling iron and organic matter transformation and bioavailability in aquatic systems.
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