Efficient removal of PFOA with an In2O3/persulfate system under solar light via the combined process of surface radicals and photogenerated holes
The environmental persistence, high toxicity and wide spread presence of perfluorooctanoic acid (PFOA) in aquatic environment urgently necessitate the development of advanced technologies to eliminate PFOA. Here, the simultaneous application of a heterogeneous In2O3 photocatalyst and homogeneous per...
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Veröffentlicht in: | Journal of hazardous materials 2022-02, Vol.423, p.127176-127176, Article 127176 |
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Sprache: | eng |
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Zusammenfassung: | The environmental persistence, high toxicity and wide spread presence of perfluorooctanoic acid (PFOA) in aquatic environment urgently necessitate the development of advanced technologies to eliminate PFOA. Here, the simultaneous application of a heterogeneous In2O3 photocatalyst and homogeneous persulfate oxidation (In2O3/PS) was demonstrated for PFOA degradation under solar light irradiation. The synergistic effect of direct hole oxidation and in-situ generated radicals, especially surface radicals, was found to contribute significantly to PFOA defluorination. Fourier infrared transform (FTIR) spectroscopy, Raman, electrochemical scanning microscope (SECM) tests and density functional theory (DFT) calculation showed that the pre-adsorption of PFOA and PS onto In2O3 surface were dramatically critical steps, which could efficiently facilitate the direct hole oxidation of PFOA, and boost PS activation to yield high surface−confined radicals, thus prompting PFOA degradation. Response surface methodology (RSM) was applied to regulate the operation parameters for PFOA defluorination. Outstanding PFOA decomposition (98.6%) and near-stoichiometric equivalents of fluorides release were achieved within illumination 10 h. An underlying mechanism for PFOA destruction was proposed via a stepwise losing CF2 unit. The In2O3/PS remediation system under solar light provides an economical, sustainable and environmentally friendly approach for complete mineralization of PFOA, displaying a promising potential for treatment of PFOA-containing water.
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•Economical remediation In2O3/PS system explored on PFOA removal under solar light.•Direct hole oxidation and surface radicals synergistically contribute to PFOA removal.•High PFOA removal efficiencies and near-stoichiometry of fluorides release realized.•DFT calculations used for monitoring the attack process of radicals toward PFOA.•RSM, SECM, radicals-quenching and spin population analysis performed. |
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ISSN: | 0304-3894 1873-3336 |
DOI: | 10.1016/j.jhazmat.2021.127176 |