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Electro-Fenton oxidation of para-aminosalicylic acid: degradation kinetics and mineralization pathway using Pt/carbon-felt and BDD/carbon-felt cells

  • Water: From Pollution to Purification
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Abstract

Degradation of a widely used antibiotic, the para-aminosalicylic acid (PAS), and mineralization of its aqueous solution was investigated by electro-Fenton process using Pt/carbon-felt and boron-doped diamond (BDD)/carbon-felt cells with applied currents in the range of 50–1000 mA. This process produces the highly oxidizing species, the hydroxyl radical (•OH), which is mainly responsible for the oxidative degradation of PAS. An absolute rate constant of 4.17 × 109 M−1 s−1 for the oxidation of PAS by ●OH was determined from the competition kinetics method. Degradation rate of PAS increased with current reaching an optimal value of 500 mA with complete disappearance of 0.1 mM PAS at 7 min using Pt/carbon-felt cell. The optimum degradation rate was reached at 300 mA for BDD/carbon-felt. The latter cell was found more efficient in total organic carbon (TOC) removal where a complete mineralization was achieved within 240 min. A multi-step mineralization process was observed with the formation of a number of aromatic intermediates, short-chain carboxylic acids, and inorganic ions. Eight aromatic intermediate products were identified using both LC-Q-ToF-MS and GC-MS techniques. These products were the result of hydroxylation of PAS followed by multiple additions of hydroxyl radicals to form polyhydroxylated derivatives. HPLC and GC/MS analyses demonstrated that extended oxidation of these intermediate products conducted to the formation of various short-chain carboxylic acids. Prolonged electrolysis resulted in a complete mineralization of PAS with the evolution of inorganic ions such as NO3 − and NH4 +. Based on the identified intermediates, carboxylic acids and inorganic ions, a plausible mineralization pathway is also deduced. The remarkably high degree of mineralization (100%) achieved by the present EF process highlights the potential application of this technique to the complete removal of salicylic acid-based pharmaceuticals from contaminated water.

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Acknowledgements

C.T. Aravindakumar is thankful to Université Paris-Est Marne-la-Vallée for a visiting professorship position.

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Authors and Affiliations

  1. Laboratoire Géomatériaux et Environnement (LGE), Université Paris-Est, EA 4508, UPEM, 77454, Marne-la-Vallée, France

    Nihal Oturan, Hugo Olvera-Vargas & Mehmet A. Oturan

  2. School of Environmental Sciences, Mahatma Gandhi University, Kottayam, Kerala, 686560, India

    Charuvila T. Aravindakumar & Mathew M. Sunil Paul

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  1. Nihal Oturan
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  2. Charuvila T. Aravindakumar
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  3. Hugo Olvera-Vargas
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  4. Mathew M. Sunil Paul
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  5. Mehmet A. Oturan
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Correspondence to Mehmet A. Oturan.

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Responsible editor: Vítor Pais Vilar

Highlights

• Degradation of para-aminosalicylic acid (PAS) by electro-Fenton (EF) process.

• Rate constant for oxidation of PAS by •OH = 4.17 × 109 M−1 s−1.

• Complete mineralization of 0.1 mM PAS solution at 240 min.

• Identification of eight aromatic intermediates by LC-Q-ToF-MS and GC-MS techniques.

• A plausible pathway for mineralization of PAS by •OH generated in EF process.

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Oturan, N., Aravindakumar, C.T., Olvera-Vargas, H. et al. Electro-Fenton oxidation of para-aminosalicylic acid: degradation kinetics and mineralization pathway using Pt/carbon-felt and BDD/carbon-felt cells. Environ Sci Pollut Res 25, 20363–20373 (2018). https://doi.org/10.1007/s11356-017-9309-6

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  • DOI: https://doi.org/10.1007/s11356-017-9309-6

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