4.5 Article

A quantitative analysis of hydroxyl radical generation as H2O2 encounters siderite: Kinetics and effect of parameters

Journal

APPLIED GEOCHEMISTRY
Volume 126, Issue -, Pages -

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.apgeochem.2021.104893

Keywords

Hydroxyl radical; Heterogeneous fenton-like reaction; Siderite; In-situ remediation

Funding

  1. National Natural Science Foundation of China [41772038]
  2. Fundamental Research Funds for the Central Universities [PA2019GDQT0009]

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The study found that under different solution chemistry conditions, siderite can activate H2O2 to produce hydroxyl radicals for the degradation of typical micropollutants. The dosage of siderite and H2O2 concentration can affect the generation of hydroxyl radicals, while the presence of different anions and metal ions also has an impact on the reaction.
Siderite is a conventional mineral of sedimentary rock and can activate H2O2 to produce hydroxyl radicals (center dot OH). Bisphenol A (BPA), 2,4-dichlorophenoxyacetic acid (2,4-D), and sodium sulfadiazine are selected as typical micropollutants to be degraded in a siderite-activated H2O2 system. To determine the influence of solution chemistry on siderite-activated Fenton-like reactions, the amount of center dot OH was quantified by using benzoic acid as a probe molecule, and then, kinetic fitting was used to analyze the reaction rate. The results showed that in the range of pH values from 3 to 9, the dissolved Fe2+ and the lattice Fe(II) of siderite activate H2O2 to generate center dot OH. An increase in siderite dosage and H2O2 concentration favored the generation of center dot OH, but higher siderite dosage and H(2)O(2 )concentration suppressed the production rate. The inhibition order of anions on the generation of center dot OH was confirmed as follows Cl- > NO3- > SO42-. Little difference was observed in the presence of Ca(2+ )and Mg2+, while the presence of Mn2+ significantly promoted the production of center dot OH. The suppression of humic acid (HA) became more serious as the HA concentration increased. Cycling experiments proved that the system could still produce center dot OH in four cycles, although the production rate experienced a slight decrease. The experimental results suggested the role of siderite in the degradation of organic pollution in the process of in-situ soil and ground-water remediation.

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