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Correlation with Fluori Science of the Total Environment 681 (2019) 497–502 Contents lists available at ScienceDirect Science of the Total Environment journal homepage: www.elsevier.com/locate/scitotenv Total arsenic and inorganic arsenic speciation in groundwater intended for human consumption in Uruguay: Correlation with fluoride, iron, manganese and sulfate Ignacio Machado a,⁎, Valery Bühl a, Nelly Mañay b a Analytical Chemistry, DEC, Faculty of Chemistry, Universidad de la República, Gral. Flores 2124, Montevideo, Uruguay b Toxicology, DEC, Faculty of Chemistry, Universidad de la República, Gral. Flores 2124, Montevideo, Uruguay HIGHLIGHTS GRAPHICAL ABSTRACT • Arsenic in groundwater is one of the main concerns of Medical Geology in Uruguay. • Analytical methodologies were devel- oped for arsenic and arsenic species as- sessment. • The validated methods were success- fully applied to the analysis of ground- water. • Arsenic levels were correlated with other relevant inorganic parameters. • These relationships should be deeply studied to prevent long-term health effects. article info abstract Article history: Medical Geology is a growing field in Uruguay and the groundwater quality has been the focus of multiple Received 22 December 2018 studies, being As levels one of its main concerns. The aim of this study was the application of analytical method- Received in revised form 7 May 2019 ologies for the assessment of total arsenic and inorganic arsenic species, fluoride, iron, manganese and sulfate in Accepted 8 May 2019 groundwater samples from private wells, used for human consumption, and to evaluate the possible correlations Available online 9 May 2019 among these parameters. The accuracy of the methods was ensured by using certified reference materials. A total Editor: Dr. Elena Paoletti of 48 groundwater samples from Uruguay were analyzed. The concentration ranges found were: tAs (1.72–120.48) μgL−1,F− (0.024–1.528) mg L−1,Fe(0.62–211.38) μgL−1 and Mn (0.11–8.705) μgL−1. Almost Keywords: half of the samples presented tAs concentration levels above those recommended by WHO for drinking water − Groundwater (10 μgL 1), with the corresponding risks for human health. Results showed higher As(V) levels in the samples, Arsenic speciation which is in agreement with the oxidant conditions of the wells. Pearson correlations were performed, resulting in Inorganic parameters − − 2− strong positive correlations for As/F , As(V)/F and As(V)/SO4 . As levels in groundwater and its relationship with other inorganic parameters, should be deeply studied to prevent long-term health effects. © 2019 Elsevier B.V. All rights reserved. 1. Introduction ⁎ Corresponding author. Uruguay is a South American country located between Argentina E-mail address: [email protected] (I. Machado). and Brazil. It is home to an estimated 3.3 million people, of whom 1.8 https://doi.org/10.1016/j.scitotenv.2019.05.107 0048-9697/© 2019 Elsevier B.V. All rights reserved. 498 I. Machado et al. / Science of the Total Environment 681 (2019) 497–502 million live in the metropolitan area of its capital and largest city, As appears with different oxidation states (-III, 0, III, V) and can be Montevideo (INE, 2011). present in inorganic and organic chemical forms. As species mostly OSE is the Uruguayan state-run utility company in charge of drinking found in groundwater are As(III) and As(V), as previously reported water supply and sanitation throughout the country. The source of (Bundschuh et al., 2008; Litter et al., 2009). In reducing aquifers, As drinking water supply to Montevideo and Canelones (most densely (III) generally constitutes a high proportion of the total As (tAs). Its mo- populated cities) is from Santa Lucía River. Only 28% of the population bilization is usually originated by desorption of mineral oxides and the receive drinking water from groundwater sources (OSE, 2018). UNIT is reductive dissolution of Fe and Mn oxides. On the other hand, in pre- the institution that establishes the regulations for drinking water qual- dominantly oxidizing environments, As(V) generally constitutes the ity parameters in Uruguay (UNIT, 2010). However, rural homes and highest proportion. This can be related to high levels of dissolved oxy- − small towns do not have water supply from OSE. In these cases, people gen, high pH values, relatively high concentrations of nitrate (NO3 ) 2− − drink water from their own wells, which sometimes are not properly and sulfate (SO4 ), often high concentrations of fluoride (F ), along + controlled. with low concentrations of ammonium (NH4 ), Fe and Mn. Since inor- The geological profile of the main Uruguayan aquifers shows great ganic As (iAs) species present different degrees of toxicity among variability due to the rocky substratum of the country, which varies them, being As(III) more toxic than As(V), it is important to carry out from sedimentary basins with good porosity and permeability, to areas speciation analysis (Smedley et al., 2001; Smedley and Kinniburgh, of crystalline basement where the water is lodged in, along with a system 2013). of interconnected faults that give rise to fissured porous aquifers. The aim of this study was the application of analytical methodolo- The Uruguayan territory can be divided into three hydrogeological gies for the determination and assessment of tAs and iAs species, F−, 2− systems according to the hydrogeological chart: Paranaense, Meridional Fe, Mn and SO4 in private wells destined for human consumption in and Costero (Collazo and Montaño, 2012). The Paranaense system oc- Uruguay, of which no systematic control studies are carried out. Also, cupies the northeast and northcentral part of the country. The most im- to evaluate the possible correlations between tAs and iAs with the men- portant aquifer of this system is the Guaraní aquifer, which represents tioned inorganic parameters. The application of speciation techniques is one of the largest freshwater reservoirs in the world, also shared with of utmost importance in Uruguay, for geochemical and toxicological Argentina, Brazil and Paraguay. Mercedes and Salto aquifers also belong studies. to this system. The Meridional system occupies most of the country sur- To the best of our knowledge, this is the first study specifically fo- face and possesses extremely changing hydrogeological characteristics. cused on the evaluation of As species and its correlation with other inor- The Costero system is formed by the Raigón aquifer, which represents ganic parameters present in groundwater in Uruguay. Thus, novel the largest reserve of underground water in the south part of the coun- information is presented from different samples collected at different try, and Chuy aquifer, which is located discontinuously on the east coast geographic points of the country. of the country (Collazo and Montaño, 2012). This work is inspired by the research interest on As levels in ground- Arsenic (As) levels in natural waters have been reported in different water sources in Uruguay, that arose in the last decade owing to the fact environments, although the highest concentrations were found in that WHO lowered the maximum recommended levels for this element groundwaters, mainly linked to natural geochemical processes in drinking water for health reasons (WHO, 2018). Also, the fact that As (Smedley and Kinniburgh, 2002), including volcanic eruptions and the is a naturally occurring element in the Earth's crust that can be released erosion of As containing minerals (Bundschuh et al., 2008). into drinking water supply sources throughout different hydrogeological As possess a high mobility and transformation capacity that makes it processes, and the high levels found in groundwaters in certain regions of easy to be slurped or desorbed from particles, and to change its oxida- the neighboring country Argentina, emerged as the research hypothesis tion state by the action of microorganisms or when reacting with oxy- for carrying out a deeper study in our country, focused on groundwater gen or other molecules present in the air, water or soil. For this samples intended for human consumption that are out of the scope of reason, it may be present in many environmental matrixes, specially the water state-run utility. The evaluation of correlations with other water (Litter et al., 2009). inorganic parameters will increase the knowledge of the geochemical dis- Medical Geology is a growing field in Uruguay and the groundwater tribution and behavior of As in groundwaters, contributing to more effi- quality has been recently the focus of multiple studies, being As risks ex- cient remediation actions. posure from drinking water, one of its main concerns. The presence of geogenic As in groundwater has been reported in publications since 2. Materials and methods 2007, showing levels above those recommended by WHO guidelines for drinking water (10 μgL−1) in several samples collected from differ- 2.1. Reagents ent aquifers (WHO, 2018). Manganelli et al. studied the main aquifers of the southwest part of the country. Elevated As concentrations were Standard solutions for calibration curves were prepared by serial di- found in Chuy (up to 41.9 μgL−1), Raigón (up to 18.9 μgL−1)and lution of commercial stock solutions (1000 mg L−1)ofAs(V),FeandMn −1 Mercedes (up to 58 μgL ) aquifers. Guérèquiz et al. and Bundschuh (Merck, Germany) in 0.1% v/v nitric acid (HNO3)preparedfromconcen- −1 et al. found As levels between 25 and 50 μgL in groundwaters from trated HNO3 (67% v/v, Merck, Germany). A commercial solution of Pd −1 San José department. Authors assumed that As occurrence in Raigón (NO3)2 (Merck, Germany) containing 10,000 mg L was used to pre- aquifer is related to continental sediments containing volcanic ashes, pare the chemical matrix modifier for As determinations by ETAAS. as in the nearby Puelche aquifer located in Buenos Aires, Argentina. A stock solution (1000 mg L−1) of As(III) was prepared by dissolu- −1 This assumption is supported by the positive correlations between As tion of sodium arsenite (NaAsO2 99.0%, Sigma-Aldrich) in 1 mol L so- contents with other trace elements, which are typical elements from dium hydroxide (NaOH 98.0%, Merck, Germany).
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