Elsevier

Science of The Total Environment

Volume 447, 1 March 2013, Pages 248-254
Science of The Total Environment

Fate and removal of typical pharmaceuticals and personal care products by three different treatment processes

https://doi.org/10.1016/j.scitotenv.2013.01.009Get rights and content

Abstract

The presence and distribution of typical of pharmaceuticals and personal care products (PPCPs), which comprise two types of polycyclic musks (PCMs) including Galaxolide (HHCB) and Tonalide (AHTN) as well as six types of estrogens containing estrone (E1), 17β-estradiol (E2), estriol (E3), 17α-ethynylestradiol (EE2), diethylstilbestrol (DES), and bisphenol A (BPA), were investigated at two wastewater treatment plants (WWTPs) in Jiangsu, China. Only raw wastewater was treated in WWTP A while WWTP B was serving an urban-industrialized area. In the influent, the concentrations of EE2 (2193–4437 ng L 1), E2 (1126–1170 ng L 1), and DES (268–421 ng L 1) were generally higher than the previously reported values, whereas the concentrations of HHCB (306–316 ng L 1), E1 (29–129 ng L 1), E3 (53 ng L 1), and BPA (26–176 ng L 1) were much lower than those reported in other previous studies. In addition, AHTN was not detected in either WWTP and E3 was not found in WWTP B. The detected processes including anaerobic/oxic process (A/O), combined orbal oxidation ditch process (C-orbal OD) and anaerobic/anoxic/anoxic/oxic membrane biological reactor (A/A/A/O-MBR) showed higher removal efficiencies for HHCB (67–71%) and EE2 (87%) than those in other previous studies. Besides, the total hydraulic retention time (HRT) ranged between 6.7 and 20.0 h, sludge retention time (SRT) ranged between 8 and 23 d, and water temperature ranged from 24.8 to 28.2 °C. The removal efficiencies for estrogens in biological processes were related to the following factors: the level of hydrophobic estrogens, the type of removal process (C-orbal OD was consistently less efficient in removing estrogens than A/O and A/A/A/O-MBR), and a high SRT or HRT (A/A/A/O-MBR with higher SRT and HRT showed higher and more stable removal of hydrophobic estrogens).

Highlights

► We investigated 8 kinds of PPCPs in each unit at 2 WWTPs with different processes. ► Agilent 1290–6460 HPLC–MS/MS was firstly utilized to detect estrogens. ► More hydrophobic estrogens such as EE2 and E2 had a higher removal efficiency. ► The OD system was less efficient than A/O and A/A/O-MBR processes in estrogen removal. ► The estrogen removal in anaerobic units was less efficient than that under aerobic conditions.

Introduction

Recent years have witnessed increasing concerns about the potential harmful consequences of exposure to micropollutants. Various non-governmental and governmental organizations such as EPA, EU, WHO, and the International Program of Chemical Safety (IPCS) are exploring problems resulting from micropollutants and setting up directives to protect and further improve the quality of water resources (Esplugas et al., 2007). Pharmaceuticals and personal care products (PPCPs), which are a group of compounds that include pharmaceutical drugs, ingredients in cosmetics, food supplements, and other personal care products such as spices, cosmetics, and their respective metabolites and transformation products (Ratola et al., 2012), are considered as such emerging microcompounds. Despite their low concentrations, PPCPs are more likely to reach and possibly accumulate in the aquatic environment because of their intrinsic properties such as high polarity and persistence (Sipma et al., 2010). Briefly, PPCPs are characterized by four prominent features. First, they consist of a wide range of compounds whose adsorption behaviors vary with each other; moreover, their behaviors are often controlled by interactions with specific functional groups or complicated external factors such as temperature, concentration and the existence of some chemical substance, resulting in difficulty in predicting their transition (Kibbey et al., 2007). Second, although their distribution is detected by the application of sophisticated modern analytical techniques, many details remain to be improved for investigating their specific properties. Third, Some PPCPs can be degraded during wastewater treatment in which the efficiencies of PPCP removal could be highly variable within and between facilities due to general operating conditions, technology used, and microbial community composition (Hedgespeth et al., 2012). Finally, they may affect water quality and potentially influence drinking water supplies, the ecosystem, and human health (Boleda et al., 2011) in ways that remain poorly understood. The effluent from wastewater treatment plants (WWTPs) is one of the most important sources of PPCPs (e.g., pharmaceuticals, personal care products, endocrine disruptors and illicit drugs) released into receiving water systems (Hedgespeth et al., 2012, Kasprzyk-Horderna et al., 2009, Grover et al., 2009, Yang et al., 2011). Thus, an emerging task that WWTPs must perform is to act as a barrier for PPCPs and prevent the emission of potentially harmful substances into the aqueous environment (Yu et al., 2013).

Polycyclic musks (PCMs) and estrogens, which are two types of representative PPCPs, are selected as the target compounds to be detected in this study. PCMs currently constitute the largest group of synthetic musks among which Galaxolide (HHCB) and Tonalide (AHTN) are the main representative compounds ranked by utilization rate (Zeng et al., 2007, Shek et al., 2008). The key structural feature of the above two musks is an indane or tetraline skeleton, which can be highly substituted by methyl groups (Ricking et al., 2003). Studies examining the toxicity of PCMs have reported a range of harmful effects. For instance, fish collected from areas all over Europe showed concentrations in the range of 0.1–1.5 μg/g wet wt. AHTN and HHCB (Schnell et al., 2009). Meanwhile, various types of estrogens, along with PCMs, have also become a public health concern because of their detrimental interference with human natural endocrine regulation (Zhang et al., 2012). Exposure of freshwater or estuarine fish to estrogens may result in the alteration of their sexual function (Labadie and Hill, 2007). For example, 4 ng L 1 of 17α-ethynylestradiol (EE2) can prevent male fathead minnows from developing normal secondary sexual characteristics (Länge et al., 2011). The natural estrogens, 17β-estradiol (E2) and its main metabolites estrone (E1) and estriol (E3), along with the synthetic estrogens such as EE2, contribute to a large extent to the estrogenicity of WWTP effluent (Xu et al., 2012). Considering that only a few studies were previously conducted on diethylstilbestrol (DES) in the wastewater treatment field and that bisphenol A (BPA) was especially widespread to an extreme degree in China (Zoeller et al., 2005), these two estrogens were also investigated in this study.

In specific area of China, few studies are focus on the efficacies of different units within a specific WWTP or how various WWTP treatment technologies compare in terms of removal of PPCPs. However, this information is important to decide appropriate steps for minimizing risk from PPCP emissions into the environment. In addition, given that most of the related researches on PPCPs have only focused on the preliminary influent and effluent at WWTPs in China, this study was conducted to illustrate the removal of PPCPs in different units at different plants using different treatment processes. Two WWTPs, located in Yangtze River and Taihu Lake, were chosen as the specific cases. In this study, HPLC–MS/MS (Agilent 1290–6460 system) was firstly used to detect the six estrogens. There was considerable ambiguity regarding the removal mechanism. Thus, this study was expected to provide greater insight into the development of wastewater treatment technologies for PPCP removal.

Section snippets

Sampling from WWTPs

WWTP A at Nanjing, with a capacity of 640,000 m3 d 1, utilizes the anaerobic/oxic process (A/O). The investigated processes of WWTP B at Wuxi are anaerobic/anoxic/anoxic/oxic membrane biological reactor (A/A/A/O-MBR, 50,000 m3 d 1, the fourth phase project) processes and the combined orbal oxidation ditch (C-orbal OD, 50,000 m3 d 1, the third phase project). An investigation revealed that the composition of influent was urban wastewater in WWTP A serving 1.6 million people, while 40% of the influent

Polycyclic musks

HHCB and AHTH originate mostly from shampoo, body wash, and detergent among which AHTN occupies a fraction of share (Roosens et al., 2007). As shown in Table 3, the average concentrations of HHCB in the influents of WWTP A and B were 316 and 306 ng L 1, respectively. In contrast, AHTN was clearly not detected in either WWTP in this study, whereas the concentrations of HHCB and AHTN in wastewater were reported to dominate those of other PCMs in previous studies (Upadhyay et al., 2011, Clara et

Conclusions

Selected PPCPs monitored in this study were removed effectively in both WWTPs and different biological techniques for wastewater treatment were compared. EE2 (2193–4437 ng L 1), E2 (1126–1170 ng L 1), and DES (268–421 ng L 1) were present in considerably high concentrations in the influents, whereas HHCB, E1, E3, and BPA were present in much lower concentrations than those reported in other previous studies. In particular, AHTN was undetectable in both WWTPs. Biodegradation was confirmed to eliminate

Acknowledgments

This study was financially supported by the National Natural Science Foundation of China (Grant No. 51208174) and the Major Science and Technology Program for Water Pollution Control and Treatment (2012ZX07506-002-2).

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