First assessment of triclosan, triclocarban and paraben mass loads at a very large regional scale: Case of Paris conurbation (France)

Highlights

• High levels of parabens, triclosan and triclocarban are found in wastewater.

• Mass loads vary from 176 to 3039 μg PE^− 1 d^− 1 for parabens.

• Mass loads vary from 26 to 762 μg PE^− 1 d^− 1 for triclosan and triclocarban.

• French mass loads vary between 11.2 and 100.7 t y^− 1 for parabens and triclosan.

Abstract

The objective of this study was to examine the occurrence of parabens (5 congeners), triclosan (TCS) and triclocarban (TCC) at the scale of the Parisian sewer network and to provide representative knowledge on these compounds in France for a large area. For this purpose and in collaboration with the Parisian public sanitation service (SIAAP) in charge of the collect and treatment of the Parisian wastewater, this study focused on seven main sewer trunks of the Paris conurbation, accounting for 1 900 000 m³ d^− 1, i.e., about 8 million inhabitants. Concentrations lying in the 2000–20 000 ng l^− 1 ranges were found in wastewater, confirming the ubiquity of parabens, TCS and TCC in our environment and household products. Parabens (> 97%) and to a lesser extent TCS (68% in median) were mainly associated to the dissolved fraction, as demonstrated by low K_D and K_OC values. For the first time, this study also evaluated the pollutant mass loads per population equivalent (PE) of parabens, TCS and TCC at the large and representative scale of the Parisian conurbation. Hence, the median mass loads varied from 176 to 3040 μg PE^− 1 d^− 1 for parabens and from 26 to 762 μg PE^− 1 d^− 1 for TCS and TCC. Based on these results and according to the assumptions done, the extrapolation of the mass loads at the national scale pointed out an annual mass loads between 51.8 and 100.7 t y^− 1 for methyl paraben (MeP) and between 11.2 and 23.5 t y^− 1 for TCS. Mass loads per equivalent habitant and national mass loads are both extremely relevant and innovative data. Contrary to other countries, such data are nowadays rather difficult to gain in France and neither enquiry nor database provides access to information on the use and production of these chemicals. Since cosmetic industries are voluntarily and fully engaged in the substitution of parabens, triclosan and triclocarban in personal care product, this study could constitute a “time reference status” which could be used as a basis for future monitoring.

Introduction

As a result of human activities and consumption of a large array of chemicals, numerous contaminants including pharmaceuticals and personnel care products (PPCPs), flame retardants, endocrine disruptors and priority pollutants as defined by the European water framework Directive are present in wastewater (Berge et al., 2013, Gasperi et al., 2008a, Kolpin et al., 2002, Lee et al., 2005, Paxeus, 1996). Among them, PPCPs are of increasing concerns owing to their ubiquities in environmental compartments, their persistent inputs, and their potential threat to environment and human health (Halling-Sorensen et al., 1998, Lee et al., 2005, Liu and Wong, 2013, Onesios et al., 2009). Among the most concerned PPCPs, preservative agents such as parabens (esters of p-hydroxybenzoic acid), triclosan (TCS, 5-chloro-2-2,4-dichlorophenoxy) and triclocarban (TCC, 3,4,4′-trichlorocarbanilide) are commonly employed in food, cosmetic (soaps, shampoos, detergents, toothpastes, etc.) and pharmaceutical products. These compounds are antiseptic, bactericidal and fungicidal agents. The esters of p-hydroxybenzoic acids with alkyl and aryl subsistent including methyl- (MeP), ethyl- (EtP), propyl- (PrP), isobutyl- (IsoBuP), butyl- (BuP) and benzyl-paraben (BzP) are mostly used in personal care products. Short chain parabens (methyl-, ethyl- and propyl-) are mainly used in liquid personal care products (liquid soap, etc.), while long chain congeners (butyl- and isobutyl-) are mostly employed in creams (Eriksson et al., 2009). According to an enquiry led by Tavares et al. (2009) in Spain on 215 personal care products, 99% of creams and 77% of cleansing lotions and make-up removers contained parabens. In France in 2009, about 7000 personal care products or formulations containing MeP were marketed against 3000–5000 products containing the remaining paraben esters (Mintel database, Global Market Research and Market Insight (Mintel, 2013)). Similarly, 860 products containing TCS were listed against only 4 containing TCC. Data on their mass loads are nevertheless not available.

For parabens, the maximum allowable concentration is 1% (w/w) (Tavares et al., 2009). According to EC Scientific Committee on Consumer Safety (SCCS) updated opinion in 2013 (SCCS, 2013), ethyl- and methyl-parabens are considered safe at a maximum concentration of 0.4% w/w for single and 0.8% w/w for mixtures of esters. Following the recent debate on the safety of the use of parabens as preservatives in cosmetics in 2013, and based on the last SCCS opinion, the European Commission (EC) decided to ban benzyl-, pentyl-, isopropyl-, isobutyl- and phenyl-parabens. The combined use of butyl- and propyl-parabens is to be limited to 0.19% w/w (as esters).

Similar to parabens, TCS is used in a large array of products including soaps, deodorants, toothpastes and can be also used as additives for plastics or food packaging and textiles whereas TCC has a more restricted use (soaps or body washes). The main application of TCS is in PPCPs (85% of total production) against 10% for textile or food packaging (Bedoux et al., 2012). Recently in 2010, the use of TCS as additive in food plastic packaging was banned by the EC 2010/169/EU. For TCS and TCC, up to 0.3% (w/w) and 5% (w/w) are respectively added to a variety of consumer products in the US (Halden and Paull, 2005).

For these compounds, a particular attention has been paid to their fate within wastewater treatment plants (WWTPs) in different areas (Gracia-Lor et al., 2012, Kasprzyk-Hordern et al., 2009, Miege et al., 2009, Sim et al., 2010). However, today, data on their production and consumption are confidential and thus rather difficult to obtain. As an alternative way, some experimental studies estimated the mass loads of triclosan and parabens in wastewater at different scales (houses, neighborhood or catchments) (Eriksson et al., 2009, Lindstrom et al., 2002, Palmquist and Hanæus, 2005, Wind et al., 2004). For parabens, only Eriksson et al. (2009) in Denmark evaluated individual paraben mass loads in graywater between 30 and 275 μg inhab^− 1 d^− 1 at the scale of 120 resident buildings. In Sweden, Palmquist and Hanaeus (2005) evaluated the load of triclosan at 200 μg per population equivalent and per day (μg PE^− 1 d^− 1) in graywater and 100 μg PE^− 1 d^− 1 in blackwater for a block of 47 small one-family houses consisting of 169 persons. At a larger scale, Lindstrom et al. (2002) reported in Switzerland triclosan mass loads at 412 μg inhab^− 1 d^− 1 (190–750 μg inhab^− 1 d^− 1) in influents from WWTPs serving populations between 4500 and 19 000 persons. In spite of these significant experimental inputs, knowledge on the occurrence and mass loads of these chemicals are deeply needed since data are rather limited for both compound families and concerned quite small areas. Due to high short-term variation in flow and pollutant concentrations, working at a too small scale can lead to potential bias to get a representative mass load evaluation. In addition, and due to the emerging concerns and the media coverage of parabens and triclosan as potential endocrine disruptors, a consumption decrease of personal care products containing parabens, TCS and TCC is expected. To date, no data show this trend and no study fixed an initial state.

In this context, this study was therefore launched as part of the OPUR (Observatory of Urban Pollutants in Paris) research program, with the objective of examining the occurrence of parabens, TCS and TCC at the scale of the Parisian sewer network and to provide representative data on these compounds in France at the scale of the Parisian conurbation. For this purpose and in collaboration with the Parisian public sanitation service (SIAAP) in charge of the collect and treatment of the Parisian wastewater, this study focused on the main seven sewer trunks of the Paris conurbation (Fig. 1). The total flow was estimated at 1 900 000 m³ d^− 1, corresponding to about 8 million inhabitants, i.e., 13% of the national population. At this scale, the objectives of the present study are i) to assess the occurrence and the concentration ranges of parabens, TCS and TCC in the Parisian wastewater, ii) to examine their partitioning between the dissolved and particulate phases, iii) to evaluate pollutant mass loads per population equivalent (PE) at a large scale area and finally iv) to extrapolate mass loads at a national scale.

By investigating the occurrence and mass loads of these chemicals at the Parisian and then at the national scales, this study delivers new and original data on the actual consumption of these chemicals in developed countries such as France. This study also provides a reference status which could be used as a basis for future monitoring and for setting sustainable policies.