Regulating >Fe(II)/>Fe(III) valence transformation in sulfite activation by oxygen vacancy enriched γ-Fe2O3 for efficient iohexol abatement

Separation and Purification Technology(2024)

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摘要
Sulfite activation with iron-based heterogeneous activators is a promising technology for the removal of organic contaminants from water. However, the slow valence transformation of >Fe(II)/>Fe(III) compromises sulfite activation efficiency. Regarding that the oxygen vacancy (Vo) can modulate the charge distribution and thus enhance >Fe(II)/>Fe(III) valence transformation via rapid electron transfer, Vo-enriched γ-Fe2O3 is constructed for sulfite activation (simplified as the γ-Fe2O3-Vo/sulfite system). The γ-Fe2O3-Vo/sulfite system exhibits excellent abatement performance for iohexol (IOX) with the efficiency as high as 90.2 % within 1 h of reaction at pH 8.5, in which sulfate radicals (SO4•−) and hydroxyl radicals (HO•) are the major species. Electrochemical and DFT calculations reveal that Vo-enriched γ-Fe2O3 possesses lower electrical impedance and the concomitant higher electron transfer efficiency. According to a series of characterizations, the enhance >Fe(II)/>Fe(III) valence transformation is confirmed to contribute to sulfite activation via the regulation of the electronic structure by the Vo. In addition, the degradation pathways of IOX are proposed by analyzing the degradation products of IOX by UPLC-QTOF-MS. Finally, the effects of different influencing factors on the degradation of IOX and the cyclic performance suggest the system shows strong resistance to interference and reusability, exhibiting superior application potential.
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关键词
γ-Fe2O3,Sulfite activation,Oxygen vacancy,Iohexol,Advanced oxidation processes
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