Development of predicted environmental concentrations to prioritize the occurrence of pharmaceuticals in rivers from Catalonia

https://doi.org/10.1016/j.scitotenv.2019.02.078Get rights and content

Highlights

  • Consumptions of 165 pharmaceuticals used by elderly people have been reported.

  • The mean total consumption of pharmaceuticals studied between 2013 and 2016 was 623 ± 3 t year−1.

  • Amoxicillin is expected to pose adverse effects for cyanobacteria.

  • Metformin pose a small potential for adverse effects to invertebrates and fish.

  • Moreover, ibuprofen also poses a small potential for adverse effects to fish.

Abstract

The main objective of the present study is to prioritize those pharmaceuticals that have higher chances to be detected in water due to incomplete removal in Wastewater Treatment Plants (WWTPs). To do so, the total consumption of pharmaceuticals in Catalonia (NE Spain) were compiled to calculate the predicted environmental concentrations (PECs) in wastewater effluents and in river water. PECs were estimated using publicly available consumption data in the period of 2013–2016 for a suite of 165 compounds. The selected compounds were based on generic pharmaceuticals with emphasis on drugs consumed by people aged 65 or over as they represent the age group with the highest consumption of pharmaceuticals. The mean total consumption of pharmaceuticals in the period studied was of 623 ± 3 t per year. Paracetamol, metformin and ibuprofen were the most administered drugs although the highest PEC values corresponded to metformin, amoxicillin and metamizole. Finally, predicted environmental levels together with acute and chronic toxicological data allowed estimating the risks of these compounds. Amoxicillin is expected to pose adverse effects for cyanobacteria, whereas metformin and ibuprofen pose a small potential for adverse effects to invertebrates and fish, respectively.

Introduction

Nowadays, water pollution represents one of the most serious ecological threats we face. Hence, quality of water has to be preserved to protect the environment and human health from compounds capable of exerting an effect at low levels of concentration. Among other chemicals, pharmaceuticals represent nowadays a relevant class of contaminants because they are continuously released into the aquatic environment and are considered as ‘pseudo-persistent’ pollutants (Daughton, 2003; Kümmerer, 2009). The first findings of pharmaceuticals in the aquatic environment were reported in the seventies, where the presence of drugs and drug metabolites were detected in sewage water effluent (Hignite and Azarnoff, 1977). Since then, the recurrent and global occurrence of pharmaceuticals in wastewater treatment plants (WWTPs) and surface waters (river, seas, lakes) is reported in the range of ng L−1 and μg L−1 (Hernando et al., 2006; Kümmerer, 2001; Navarro-Ortega et al., 2012a; Navarro-Ortega et al., 2012b; Ternes et al., 2001). Human consumption, animal use, waste disposal and/or manufacturing are the main sources of pharmaceuticals to the environment (Daouk et al., 2015).

Regarding human consumption, the drugbank has 11,901 drugs in its database (Wishart et al., 2018) and the European Medical Agency (EMA) compiles around 2500 active ingredients. Consumption of pharmaceuticals by the global population varies among countries and its use is expected to grow as the population ages and upon polimedication. Virtually every country in the world is experiencing growth in the number and proportion of the elder population. In 2017, 962 million people aged 60 or over were estimated at a global scale, comprising 13% of the global population, and raising to 25% in Europe. This age group is growing at a rate of about 3% per year (United Nations (UN), 2015). Elder population in developed countries have a high consumption of pharmaceuticals (Valderrama Gama et al., 1998), Typical consumption of 5–10 pills/patient/day in residents of senior residences which is translated in a total consumption of pharmaceuticals of hundreds of milligrams per day/person (Lacorte et al., 2017).

Because monitoring of all pharmaceuticals consumed is practically impossible in terms of time and cost, prioritization tools are needed for compounds that deem to pose negative effects in the environment. Predicted environmental concentrations (PECs) is a practical way (Carballa et al., 2008; Franquet-Griell et al., 2015), to estimate the concentrations of drugs expected to be found in the environment based on consumption data. Its use has been reported before for cytostatic (Franquet-Griell et al., 2015; Franquet-Griell et al., 2017) and other drugs (Burns et al., 2018; Guo et al., 2016; Verlicchi et al., 2014) in wastewater and surface waters.

On the other hand, many pharmaceuticals have been reported to be acutely and chronically toxic to aquatic biota with effects varying largely across taxa and among chemical groups (Crane et al., 2006; Fent et al., 2006a; Overturf et al., 2015; Owen et al., 2007; Santos et al., 2010). Acute toxicity values (immobilization or mortality, algae growth within 48–96 h and the half-maximum effective concentration or lethal concentration, EC50/LC50, value) of pharmaceuticals to algae, aquatic plants, Daphnia magna and fish species have been generally reported in the order of mg L−1. Moreover, in terms of chronic toxicity, most individual pharmaceuticals (such as antibiotics, antibacterial drugs, anti-inflammatory drugs, non-steroidal anti-inflammatory drugs) induce reproductive toxicity in fish and crustaceans at low or environmentally relevant concentrations (ng L−1-μg L−1) (Crane et al., 2006; Fent et al., 2006a; Overturf et al., 2015; Owen et al., 2007; Santos et al., 2010). In addition, the combination of different drugs sharing a common mechanism of action could produce additive effects that would be enough to enhance toxicity (Cleuvers, 2004; Fent et al., 2006b).

Taking into account the large amount and diversity of pharmaceuticals consumed and discharged to the environment, the aim of this study was to prioritize and evaluate their environmental risk by calculating PECs according to the consumption in hospitals and pharmacies from 2013 to 2016. The procedure has been optimized considering Catalonia, a region of 7.5 million inhabitants, with an elderly population (≥65 years) of 24.5%. This region suffers from water scarcity and thus, the levels and potential toxic effects of pharmaceuticals can be high. PECs were calculated in 11 river basins according to specific population distribution and dilution factor (DF). In addition, the potential risk for the aquatic environment was studied considering acute and chronic toxicity of different aquatic taxa for selected pharmaceuticals with highest PECriver.

Section snippets

Consumption data

Consumption data, being the term “consumption” the dispensation or sales of pharmaceuticals, were obtained from Catalan Health Service (CatSalut) over the period 2013–2016 in pharmacies and hospitals. Compound selection was based on medical prescriptions for the elderly (>65 years) in Catalonia in the last years (http://observatorisalut.gencat.cat) (Generalitat de Catalunya - Catalan Health System Observatory, 2018). A total of 165 drugs belonging to 13 different Anatomical Therapeutic

Consumption of pharmaceuticals: the case study of Catalonia

The mean total consumption of 165 pharmaceuticals in the four years studied (2013–2016) was 623 ± 3 t per year (Table SI2). In 2013, the total consumption of these pharmaceuticals was 599 t year−1, increasing up to 638 t year−1 in 2016, showing a 6.5% increase. ATC groups N (nervous system), A (alimentary tract and metabolism) and M (musculo-skeletal system) showed the highest consumptions with values between 47 and 318 t year−1 respectively. Fig. 1 displays the consumption trends for all

Conclusions

This study reveals the importance of consumption data and temporal patterns for estimating the occurrence and risk of pharmaceuticals consumed by elderly people in surface waters. An extensive data compilation on pharmaceuticals consumption in Catalonia was performed. The mean total consumption of these pharmaceuticals in the period studied (2013–2016) was 623 ± 3 t per year. ATC groups N (nervous system), A (alimentary tract and metabolism) and M (musculo-skeletal system) showed the highest

Acknowledgments

The authors wish to thank CatSalut, and especially Pere Carbonell and Montserrat Bosch, for kindly providing the consumption data of pharmaceuticals in Catalonia. The authors also gratefully acknowledge Teresa Sala-Comorera for helping in the initial calculations of PECs. This study has been financed by the SUDOE program with the project Innovec'Eau (2016–2019)/Project SOE1/P1/F0173 Interreg SUDOE funded by FEDER: 1.177.875,64 €; http://innovec-eau.univ-perp.fr.

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