4.8 Article

Experimental and modeling evidence of hydroxyl radical production in iron electrocoagulation as a new mechanism for contaminant transformation in bicarbonate electrolyte

Journal

WATER RESEARCH
Volume 220, Issue -, Pages -

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.watres.2022.118662

Keywords

Iron electrocoagulation; Hydroxyl radical; Adsorbed Fe(II) oxidation; Kinetic modeling; Bicarbonate

Funding

  1. Strategic Priority Research Program of Chinese Academy of Sciences [XDB40020000]
  2. National Natural Science Foundation of China [51808415, 42177237, U1612441]
  3. Science and Technology Planning Project of Guizhou Province [2022-217, 20214028]

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Iron electrocoagulation is an effective method for water purification, and recent studies have shown that it can produce hydroxyl radicals (OH-) for the oxidation of organic contaminants. However, the mechanism of OH- production in bicarbonate electrolyte is still unclear. This study found that OH- was produced during iron electrocoagulation in bicarbonate electrolyte under pH-neutral conditions, with the highest yield observed at pH 8.5. The presence of Fe(II) and lepidocrocite were also found to play a role in enhancing OH- production. A kinetic model was developed to describe the production of OH-, Fe(II) oxidation, and contaminant degradation processes in iron electrocoagulation. These findings expand the functionality of electrocoagulation and provide insights for the development of sustainable water purification technology.
Iron electrocoagulation is designed for sustainable high-efficiency and high-flexibility water purification applications. Recent advances reported that hydroxyl radicals (center dot OH)-based oxidative transformation of organic contaminants can occur in iron electrocoagulation. However, there is still a lack of mechanistic understanding the production of center dot OH in bicarbonate electrolyte, which presents a critical knowledge gap in the optimization of iron electrocoagulation technology towards practical application. Combined with contaminant degradation, radical quenching experiments, and spectroscopic techniques, we found that center dot OH was produced at rate of 16.1 mu M center dot h - 1 during 30-mA iron electrocoagulation in bicarbonate electrolyte through activation of O2 by Fe(II) under pH-neutral conditions. High yield of center dot OH occurred at pH 8.5, likely due to high adsorbed Fe(II) that can activate O2 to enhance center dot OH production. Mo center dot ssbauer and X-ray photoelectron spectroscopy measurements substantiated that Fe(II)-adsorbed lepidocrocite was the dominant solid Fe(II) species at pH 8.5. A process-based kinetic modeling was developed to describe the dynamic of center dot OH production, Fe(II) oxidation, and contaminant degradation processes in iron electrocoagulation. Findings of this study extend the functionality of electrocoagulation from phase separation to center dot OH-based advanced oxidation process, which provides a new perspective for the development of electrocoagulation-based next generation sustainable water purification technology.

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