Advanced oxidation of antihypertensives losartan and valsartan by photo-electro-Fenton at near-neutral pH using natural organic acids and a dimensional stable anode-gas diffusion electrode (DSA-GDE) system under light emission diode (LED) lighting
In this work photo-electro-Fenton (PEF) processes using a dimensionally stable anode-gas diffusion electrode (DSA-GDE) system under light emission diodes (LED)-type radiation were used in the degradation of the angiotensin-II-receptor antagonists (ARA II), valsartan (VAL), and losartan (LOS), which are used in the treatment of hypertension diseases, and are considered among the emerging contaminants (ECs). Organic acids as citric, tartaric, and oxalic acids were used as complexing agents of iron ions in order to maintain the performance of the Fenton reaction at near-neutral pH value. The results show that at 3.42 mA/cm2 after 90 min of electro-Fenton (EF) treatment, degradation of 70% of VAL and 100% of LOS were observed. Total degradation of VAL and LOS was reached with a PEF process at the same time with mineralization of 30%. When citric and tartaric acids were used instead of oxalic acid, similar results were obtained, i.e., total degradation of both compounds, LOS and VAL, after 90 min of treatment. The degradation performance can be attributed to the increase of the initial dissolved iron in the system, facilitating the Fe3+/Fe2+ turnover in the catalytic photo-Fenton reaction and consequently, hydroxyl radical (•OH) production. In addition, the increased photo-activity of the complexes can be associated with their high capability to complex Fe3+ and to promote ligand-to-metal charge transfer, which is of key importance to feed Fe2+ to the Fenton process. The results show that the system evaluated was more efficient to eliminate sartan family compounds using LED lighting in comparison with traditional UV-A lamps used in this kind of work. Moreover, three transformation products of VAL degradation and two transformation products of LOS degradation were identified by high-resolution mass spectrometry (HRMS) using hybrid quadrupole-time-of-flight (QTOF) MS and, at the end of the PEF system, the several organic compounds accumulated and no mineralized were effectively treated in a subsequent aerobic biological system.
KeywordsElectro-Fenton Photo-electro-Fenton Photo-electro-Fenton with organic acids Emerging contaminants Sartans Wastewater treatment Losartan Valsartan
The authors acknowledge the financial support from COLCIENCIAS (project code 111571149790). Martínez–Pachón, D. thanks Universidad Antonio Nariño for her Ph.D. scholarship (Convocatoria PFAN 2015). We also thank María Ibañez and Félix Hernández from Research Institute for Pesticides and Water (IUPA), University Jaume I, Castellón, Spain, for his contribution in the mass spectrums analysis.
- Bijlsma L, Botero-Coy AM, Rincón RJ, Peñuela GA, Hernández F (2016) Estimation of illicit drug use in the main cities of Colombia by means of urban wastewater analysis. Sci Total Environ 565:984–993Google Scholar
- De Luna MDG, Veciana ML, Su CC, Lu MC (2012) Acetaminophen degradation by electro-Fenton and photoelectro-Fenton using a double cathode electrochemical cell. J Hazard Mater 217–218:200–207Google Scholar
- Hernández F, Ibáñez M, Botero-Coy AM, Bade R, Bustos-López MC, Rincón J, Moncayo A, Bijlsma L (2015) LC-QTOF MS screening of more than 1,000 licit and illicit drugs and their metabolites in wastewater and surface waters from the area of Bogotá, Colombia. Anal Bioanal Chem 407(21):6405–6416CrossRefGoogle Scholar
- Hiltunen T, Donner K, Antti-pekka S, Saarela J, Ripatti S, Chapman A, Gums J, Gong Y, Cooper-Dhoff R, Frau F, Glorioso V, Zaninello R, Salvi E, Glorioso N, Boerwinkle E, Turner S, Johnson J, Kontula K (2015) Pharmacogenomics of hypertension: a genome-wide, placebo-controlled cross-over study, using four classes of antihypertensive drugs. J Am Heart Assoc 4(1):e001521–e001521CrossRefGoogle Scholar
- Isarain-Chávez E, Cabot PL, Centellas F, Rodríguez RM, Arias C, Garrido JA, Brillas E (2011) Electro-Fenton and photoelectro-Fenton degradations of the drug beta-blocker propranolol using a Pt anode: identification and evolution of oxidation products. J Hazard Mater 185(2–3):1228–1235CrossRefGoogle Scholar
- Martínez-Pachón D (2018) Sistemas Electro-Fenton y Foto Electro-Fenton como Método de Eliminación de Contaminantes Emergentes Presentes en aguas Residuales (Doctoral Thesis). Universidad Antonio Nariño, Bogotá D.C., ColombiaGoogle Scholar
- Panizza M (2010) Importance of electrode material in the electrochemical treatment of wastewater containing organic pollutants. In: Comninellis C, Chen G (eds) Electrochemistry for the environment. Springer, New York, pp 25–54Google Scholar
- Stumm W, and James JM (1996 Third environmental science and technology. Aquatic chemistry: chemical equilibria and rates in natural watersGoogle Scholar
- Vargas-Hernández C, Rengifo-Morocho MA (2012) Caracterización óptica de Diodos emisores de Luz mediante su espectros de emisión y patrones de radiación. Scientia et technica 2(51):66–70. https://doi.org/10.22517/23447214.7161
- Villegas- Guzman P, Giannakis S, Rtimi S, Grandjean D, Bensimon M, De Alencastro LF, Torres-Palma RA, Pulgarin C (2017) A green solar photo-Fenton process for the elimination of bacteria and micropollutants in municipal wastewater treatment using mineral iron and natural organic acids. Appl Catal B Environ 219:538–549CrossRefGoogle Scholar