Abstract
One of the main challenges of electrochemical Fenton-based processes is the treatment of organic pollutants at near-neutral pH. As a potential approach to this problem, this work addresses the use of a low content of soluble chelated metal catalyst, formed between Fe(III) and ethylenediamine-N,N'-disuccinic (EDDS) acid (1:1), to degrade the herbicide triclopyr in 0.050 M Na2SO4 solutions at pH 7.0 by photoelectro-Fenton with UVA light or sunlight (PEF and SPEF, respectively). Comparison with electro-Fenton treatments revealed the crucial role of the photo-Fenton-like reaction, since this promoted the production of soluble Fe(II) that enhanced the pesticide removal. Hydroxyl radicals formed at the anode surface and in the bulk were the main oxidants. A boron-doped diamond (BDD) anode yielded a greater mineralization than an IrO2-based one, at the expense of reduced cost-effectiveness. The effect of catalyst concentration and current density on the performance of PEF with BDD was examined. The PEF trials in 0.25 mM Na2SO4 + 0.35 mM NaCl medium showed a large influence of generated active chlorine as oxidant, being IrO2 more suitable than RuO2 and BDD. In SPEF with BDD, the higher light intensity from solar photons accelerated the removal of the catalyst and triclopyr, with small effect on mineralization. A plausible route for the herbicide degradation by Fe(III)–EDDS-catalyzed PEF and SPEF is finally proposed based on detected byproducts: three heteroaromatic and four linear N-aliphatic compounds, formamide, and tartronic and oxamic acids.
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The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.
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Funding
The authors thank the financial support from projects CTQ2016-78616-R (AEI/FEDER, EU), PID2019-109291RB-I00 (AEI, Spain), CNPq – 439344/2018-2 (Conselho Nacional de Desenvolvimento Científico e Tecnológico, Brazil), and FAPESP project 2014/50945-4 (Fundação de Amparo à Pesquisa do Estado de São Paulo, Brazil), as well as the PhD scholarships awarded to I.C. Da Costa Soares (CNPq 200009/2018-4, Brazil), Z. Ye (State Scholarship Fund, CSC, China), and R. Oriol (MINECO, Spain).
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Conceptualization: Z.H. Ye and I. Sirés. Formal analysis and investigation: I.C. Da Costa Soares, Z.H. Ye, and R. Oriol. Funding acquisition: I. Sirés, P.L. Cabot, and C.A. Martínez-Huitle. Methodology: Z.H. Ye and I. Sirés. Resources: I. Sirés and E. Brillas. Supervision: I. Sirés and C.A. Martínez-Huitle. Writing—original draft preparation: I. Sirés and E. Brillas. Writing review and editing: all authors read and approved the final manuscript.
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Da Costa Soares, I.C., Oriol, R., Ye, Z. et al. Photoelectro-Fenton treatment of pesticide triclopyr at neutral pH using Fe(III)–EDDS under UVA light or sunlight. Environ Sci Pollut Res 28, 23833–23848 (2021). https://doi.org/10.1007/s11356-020-11421-8
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DOI: https://doi.org/10.1007/s11356-020-11421-8