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  • 7/21/2019 Simultaneous Determination and Assessment of 4-Nonylphenol, Bisphenol a And

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    Simultaneous determination and assessment of 4-nonylphenol, bisphenol A andtriclosan in tap water, bottled water and baby bottles

    Xu Li, Guang-Guo Ying , Hao-Chang Su, Xiao-Bing Yang, Li Wang

    State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China

    a b s t r a c ta r t i c l e i n f o

    Article history:

    Received 9 June 2009

    Accepted 14 April 2010Available online 7 May 2010

    Keywords:

    Contaminants

    Drinking water

    Baby bottle

    Endocrine disrupting chemicals

    Risk

    This study investigated the levels of 4-nonylphenol (4-NP), bisphenol A (BPA) and triclosan (TCS) in bottled

    water and tap water in Guangzhou and release of these chemicals from baby bottles using gas

    chromatographymass spectrometry with negative chemical ionization. Results show that 4-NP was present

    in all the bottled water while 17 out of 21 contained BPA and 18 out of 21 contained TCS. Their

    concentrations in bottled water ranged from 108 to 298 ng/L, 17.6 to 324 ng/L and 0.6 to 9.7 ng/L,

    respectively. Five of the tap water samples from six drinking water plants were found to contain 4-NP and

    BPA both in June and December, while TCS was detected in the same ve plants only in June. The highest

    concentrations in tap water for 4-NP, BPA and TCS were 1987, 317 and 14.5 ng/L, respectively. Daily intakes

    of 4-NP, BPA and TCS of adults by drinking 2 L of tap water were estimated to be 1410, 148 and 10 ng/day,

    respectively. BPA was found to be released within 24 h from four brands of baby bottles at room temperature

    (24 C), 40 C and 100 C. Increased temperature led to higher release of BPA from the baby bottles.

    Estimated daily intakes of 4-NP, BPA and TCS for infants were 705, 1340 and 5 ng/day, respectively, by

    drinking 1 L of tap water from a baby bottle at 40 C. This study showed that the exposure to the three

    compounds from drinking water is unlikely to pose a health risk.

    2010 Elsevier Ltd. All rights reserved.

    1. Introduction

    In the last decades, 4-nonylphenol (4-NP), bisphenol A (BPA) and

    triclosan (TCS) attracted a lot of attention due to their potential

    endocrine disrupting effects on, or toxicity to wildlife as well as their

    human health concerns (Alexander et al., 1988; Yokota et al., 2001;

    Orvos et al., 2002; Rule et al., 2005; Ying, 2006; Fiss et al., 2007; Soares

    et al., 2008; Uchiyama et al., 2008; Yang et al., 2008). These three

    chemicals have been widely used in domestic products such as

    surfactants and food packaging lms for 4-NP (White et al., 1994;

    Khim et al., 1999; Guenther et al., 2002; Ying et al., 2002; Gatidou et al.,

    2007; Uchiyama et al., 2008), polycarbonates (PC) and epoxy resins

    products (such as baby bottles and food containers) forBPA (Olea et al.,

    1996; Biles et al., 1997; Vandenberg et al., 2007), and personal care

    products (such as toothpaste, cosmetics, skin care creams and lotions,

    soaps and dental products) for TCS (Jones et al., 2000; McAvoy et al.,

    2002; Tsai et al., 2008). It is therefore necessary to understand human

    exposure to these chemicals through consumer products.

    There are various routes of human exposure to the three

    chemicals, especially through consumption of food and water.

    Previous studies reported presence of 4-NP, BPA and TCS in human

    milk and food (Ademollo et al., 2008; Allmyr et al., 2006, 2008;

    Ballesteros-Gmez et al., 2009; Canosa et al., 2008; Dayan, 2007;

    Guenther et al., 2002; Lu et al., 2007).Ademollo et al. (2008)pointed

    out that levels of 4-NP in breast milk were related to sh

    consumption. High concentrations of 4-NP have been reported in

    seafood from Italy (Ferrara et al., 2005, 2008).Guenther et al. (2002)

    and Lu et al. (2007) indicated that 4-NP is ubiquitous in food products

    and one of the sources was found to be polyvinyl chloride (PVC) lms

    for food packaging from which 4-NP migrated into foodstuffs (Inoue

    et al., 2001; Loyo-Rosales et al., 2004).

    A recent study has suggested that the primary route for human

    exposure to BPA is through contaminated foods and beverages (Kang

    et al., 2006). In addition, BPA could leach out from many consumer

    products containers (baby bottles, epoxy resins and other consumer

    plastics) under normaluse conditions (Vandenberg et al., 2007; Leet al.,

    2008). Although BPA has been shown to have estrogenic potency and it

    may increase cancer susceptibility through developmental reprogram-

    ming (Keri et al., 2007), there has been an ongoing debate about its

    adverse endocrine disruptive effect on humans (Kang et al., 2006).

    TCS is regarded as a potential weak androgenic compound ( Foran

    et al., 2000) and its metabolite a weak estrogenic compound

    (Ishibashi et al., 2004). The dominant source of exposure to TCS was

    demonstrated to be personal care products containing TCS (Allmyr

    et al., 2006). Although adverse effects of TCS have not been

    established in humans, research is still needed to understand various

    sources of TCS due to its high-volume usage in many personal care

    products.

    Environment International 36 (2010) 557562

    Corresponding author. Tel./fax: +86 20 85290200.

    E-mail address:[email protected](G.-G. Ying).

    0160-4120/$ see front matter 2010 Elsevier Ltd. All rights reserved.

    doi:10.1016/j.envint.2010.04.009

    Contents lists available at ScienceDirect

    Environment International

    j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / e n v i n t

    mailto:[email protected]://dx.doi.org/10.1016/j.envint.2010.04.009http://www.sciencedirect.com/science/journal/01604120http://www.sciencedirect.com/science/journal/01604120http://dx.doi.org/10.1016/j.envint.2010.04.009mailto:[email protected]
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    There have also been many reports on the occurrence of these

    three compounds in surface water around the world (e.g. Kolpinet al.,

    2002; Lindstrm et al., 2002; Staples et al., 1998; Ying et al., 2002;

    Zhao et al., 2009); however, little has been done on the exposure of

    these three compounds through drinking water.

    The aim of this study was to estimate daily intakes of the target

    compounds (4-NP, BPA and TCS) by drinking water for both adults and

    infants. Weinvestigatedlevels of 4-NP, BPAand TCSin bottledwaterand

    tap water available in Guangzhou, South China. Besides adults, infantsneed more attention based on a recentstudythat infants areparticularly

    susceptible to water contaminants (Levallois et al., 2008). Thus this

    study also evaluated 4-NP, BPA and TCS migration from baby bottles as

    well. A simultaneous extraction and analysis method using gas

    chromatographymass spectrometry with negative chemical ionization

    (GC-NCI-MS) was developed to determine the concentrations of 4-NP,

    BPA and TCSin drinking water and their leaching into water fromnewly

    purchased baby bottles.

    2. Materials and methods

    2.1. Standards and reagents

    Chemical standards 4-nonylphenol (4-NP), bisphenol-A (BPA),triclosan (TCS) were obtained from Dr. Ehrenstorfer GmbH (Germany)

    or Supelco (USA), whereas 4-n-nonylphenol (4-n-NP), [2H16] bisphe-

    nol-A (BPA-d16), 13C-labelled triclosan (13C-TCS) used as internal

    standards were obtained from Dr. Ehrenstorfer GmbH (Germany),

    Supelco (USA), and Cambridge Isotope Laboratories Incorporation

    (Massachusetts, USA), respectively. Detailed information about these

    standards is listed in Table 1. The derivatization reagent pentauor-

    obenzoyl chloride (PFBOCl, purity N99%) was obtained from Aldrich.

    Solvents methanol,n-hexane, toluene, ethyl acetate, dichloromethane

    (DCM) and pyridine (HPLC-grade) were purchased from Merck

    Corporation (Shanghai, China). Supelclean ENVI-18 solid phase extrac-

    tion cartridges (500 mg, 3 ml) were purchased from Supelco Corpora-

    tion.To avoid the contamination of 4-NP, BPA and TCS, no plastics were

    allowed to be used in the experiment, and all glassware was baked for

    4 h at 400 C before use. Stock solutionsof the standards were prepared

    at 100 mg/L in methanol and stored in amber glass bottles at18 C for

    later use. The working solution of the derivatization reagent 2% (v/v) of

    PFBOCl was prepared by diluting pure derivatization reagents with

    toluene, which was kept in a glass desiccator to prevent quality

    deterioration due to moisture in the air.

    2.2. Sample collection and preparation

    Twenty-one brands of bottled water including mineral water and

    pure drinking water were purchased from a local supermarket in

    Guangzhou. They were stored unopened at room temperature(RT) until

    extraction. Tap-water samples (1 L each) were collected from six local

    residential houses, representing 6 different drinking water supplyplants of Guangzhou, andthe sites were chosento be close to thenearest

    plants. 50 mL of HPLC-grade methanol and 400L of 4 M H2SO4wereadded to the tap water samples collected in amber glass bottles

    immediately. In addition, they were transported in coolers and stored in

    a cold room at 4 C until analysis. For each brand of bottled water and all

    the tap water, three replicates were sampled and analyzed. Moreover,

    procedural blanksand spikeswere included for each batch of samples as

    quality control.

    Migration of the three compounds from baby bottles was investi-

    gated at three different temperatures (24 C, 40 C and 100 C) after24 h. Four commonly used brandsof PC baby bottles (B1, B2, B3 and B4)

    were purchased from a local supermarket in Guangzhou. The volume of

    all the baby bottles was 240 mL. For each sample, 240 mL of Milli-Q

    grade water wasaddedto each bottleand thebaby bottles were thenput

    in water baths at 24 C, 40 C and 100 C. For the experiment under the

    condition of 100 C, the baby bottles were immersed in boiling Milli-Q

    grade water only for 1 h and then kept at room temperature for 24 h.

    Then thesamples (240 mL each)were transferred to amber glass bottles

    for solid phase extraction. Time effect on migration was also

    investigated by continuously monitoring the release of BPA under

    normaluseconditions at24 C and 40 C. Onday 1,day 3,day5 and day

    7, 240 mL water samples were all transferred to amber glass bottles for

    solid phaseextraction andthen another 240 mL Milli-Q grade water was

    added to the same babybottleimmediately. For all these conditions, the

    baby bottles were wrapped in aluminum foil to avoid photolysis due to

    exposure to light. Three replicate baby bottles of each brand were used

    during the experiments. Procedural blanks were included in the

    extraction as well.

    2.3. Solid phase extraction

    Before extraction, the pH value of each water sample was

    adjusted to 3 using 4 M H2SO4and 50 mL of HPLC-grade methanol

    was added into the water to increase extraction efciency. And

    100L each of 1 mg/L of 4-n-NP, BPA-d16and 13C-TCS were spiked

    into each sample as internal standards. The cartridges were

    conditioned by 10 mL of methanol and 10 mL of Milli-Q water.

    Then water samples passed through the SPE cartridges at a ow rate

    of 10 mL/min. In order to remove any interference, sample bottles

    were rinsed with 2 50 mL of 5% (v/v) methanol in Milli-Q water

    that also passed through SPE cartridges. After loading of the

    samples, the cartridges were dried under vacuum for 2 h. The

    analytes were eluted from the cartridges using 8 mL ethyl acetate.

    The eluates were concentrated to dryness under a gentle stream of

    nitrogen, and then redissolved in methanol to a nal volume of

    1 mL. Each nal extract was ltered through a 0.45m membranelter into a 2 mL amber glass vial and kept at 18 C until analysis.

    2.4. Derivatization

    The method of derivatization was carried out based on previously

    reported methods (Boitsov et al., 2004; Zhao et al., 2009). Theprocedure was operated using a 10 ml glass tube (KIMAX, USA) with a

    Table 1

    Parameters of the target compounds and selected ions in GC-NCI-MS.

    Compoundsa Supplier M.W.c R.T. (min)c Ionsb

    4-n-NP (I.S.) c Dr. Ehrenstorfer 220 19.04 414.1 415.0 416.0

    4-NP Dr. Ehrenstorfer 220 17.63 414.1 415.0 416.0

    BPA-d16(I.S.) Supelco 244 25.51 630.0 630.9 420.1

    BPA Supelco 228 25.62 616.0 617.0 405.913C12-TCS (I.S.) Cambridge 301.5 20.41 494.0 495.8 298.9 300.8

    TCS Dr. Ehrenstorfer 289.5 20.42 484.8 483.8 286.8 288.8

    a 4-NP: 4-nonylphenol; BPA: bisphenol-A; TCS: triclosan.b The underlined ions are the ones used for quantication.c

    I.S.: internal standard; M.W.: molecular weight; R.T.: retention time.

    558 X. Li et al. / Environment International 36 (2010) 557562

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    polytetrauoroethylene (PTFE) screw cap. Firstly, 100L of the nalextract in methanol was transferred to the test tube and the solvent

    was dried under a gentle nitrogen stream. Secondly, 2 mL of 1 M

    NaHCO3 and 1 mL of 1 M NaOH were added. After shaking for 30 s,

    2 ml ofn-hexane, 50L of 10% pyridine in toluene and 50L of 2%PFBOCl in toluene were added. The tube was tightly capped and hand

    shaken violently for 1 min. After the organic phase and aqueous phase

    were separated thoroughly, the organic phase was transferred to a

    5 mL glass centrifugal tube using a glass pipette. Thirdly, 2 mL ofn-hexane was added to the 10 mL tube for a second extraction. The tube

    was hand shaken for 1 min, and the other procedures were the same

    as in the second step. After separated, the supernatant wastransferred

    to the aforementioned5 mL glass centrifugal tube. Then the combined

    n-hexane mixture was dried under a gentle nitrogen stream. Finally,

    the extract was re-dissolved in 100L of n-hexane, and thentransferred to a 2 mL amber glass vial with a 250L at-bottomed

    insert, which was ready for GC-NCI-MS analysis.

    2.5. Analysis

    GC-MS analysis of the derivatized samples was carried out using

    an Agilent 6890 N gas chromatograph connected to an Agilent 5975B

    MSD mass spectrometer with a chemical ionization (CI) source

    (Agilent, USA). The target compounds were separated on a capillary

    column DB5-MS (30 m0.25 mm, 0.25m lm thickness). Heliumwas used as the carrier gas and maintained at a constant ow rate of

    1.0 mL/min, and the reaction gas was high-purity methane

    (N99.999%) with a constant ow of 2.0 mL/min. The temperatures of

    both ion source and quadrupole were set at 150 C. A sample volume

    of 1L wasinjected in splitless mode at an inlet temperature of 300 C.The GC oven temperature program applied was as follows: from 80 C

    (1 min) to 220 C at 10 C/min, from 220 C to 260 C at 4 C/min, and

    from 260 C to 300 C (8 min) at 5 C /min, then to the temperature of

    310 C (15 min) at 20 C /min. The MS interface temperature was

    maintained at 310 C. The characteristic ion fragments of the

    derivatized 4-NP, BPA and TCS were selected for quantication and

    conrmation under selected ion monitoring mode (Table 1).

    2.6. Validation of the method

    The recoveries of the analytes using this analytical method were

    tested in four replicates by spiking 5 ng, 100 ng, and 200 ng of each

    analyte standard to 1 L of surface water collected from the Liuxi

    Reservoir. Twoprocedural blankswere included at the same time. The

    recoveries of each target compound at the three spiking levels were

    ranged from 74% to 118% (Table 2). The limit of detection (LOD) and

    limit of quantitation (LOQ) of each compound were determined

    respectively as three times and ten times the standard derivations

    (SD) of seven replicates of the spiked water at the concentration of

    5 ng/L. The LOD values for 4-NP, BPA and TCS were set at 2.0, 0.7 and0.2 ng/L, while the LOQ values were 7.0, 2.0 and 0.5 ng/L, respectively.

    3. Results and discussion

    3.1. Bottled water

    Table 3lists the concentrations of each compound detected in bottled drinking

    water of 21 brands in the market. The detection rate of 4-NP, BPA and TCS was 100%,

    81% and 86%, respectively. Concentrations of 4-NP, BPA and TCS ranged from 108 to

    298 ng/L, 17.6 to 324 ng/L and 0.6 to 9.7 ng/L, respectively. Among the three target

    compounds, 4-NP hadthe highestaverage concentration and TCS hadthe lowest, while

    the concentrations of BPA varied the most.

    3.2. Tap water

    The concentrations of 4-NP, BPA and TCS in tap water from the six drinking water

    plants were listed in Table 4. In the June sampling, the three target compounds were all

    detected inthe six drinking water plants except forPlant 6 without TCS being detected,

    and the highest concentrations of all the three target compounds were 1070 ng/L for 4-

    NP, 317 ng/L for BPA and 14.5 ng/L for TCS, which was found in Plant 5. The

    concentrations of 4-NP in tap-water samples were the highest among the three target

    compounds, ranging from 196 to 1070 ng/L. As for BPA, the concentration varies a lot

    from 2.3 to 317 ng/L. The concentrations of TCS ranged from below the LOQ to 14.5 ng/

    L. In the December sampling, 4-NP and BPA were detected with concentrations up to

    1990 ng/L for 4-NP and 123 ng/L for BPA, but no TCS was detected in all six plants.

    3.3. Baby bottles

    This study showed that BPA was released from the baby bottles at RT (24 C), 40 C

    and 100 C (Table 5). Temperature affected the migration of BPA from baby bottles to a

    certain degree, with BPA released signicantly at 100 C. The highest migration of BPA

    was found in Brand 3, and the amount released into the water were 267, 987 and

    4500 ng at 24 C, 40 C and 100 C within the rst 24 h. The lowest migration of BPA

    was found in Brand 1 and Brand 4. No signicant 4-NP and TCS were found released

    from the baby bottles at the three temperatures.

    Table 6 shows that BPAmigratedout continuously into water from thebaby bottles

    under normal use conditions at 24 C and 40 C. The amount of BPA released from the

    baby bottles in the following days was lower than that of the rst day.

    4. Discussion

    Drinking water is an important route of human exposure to

    contaminants including 4-NP, BPA and TCS. Trace levels of these

    chemicals were detected in bottled water from a local supermarket in

    Guangzhou. The concentration of 4-NP in the bottled water of this

    Table 2

    Recoveries (%) and limits of detection of the target compounds.

    Compoundsa Spiked concentrationsb LOD

    (ng/L)cLOQ

    (ng/L)c5 ng/L 100 ng/L 200 ng/L

    4-NP 92 4 115 13 74 5 2.0 7.0

    BPA 118 8 103 1 105 3 0.7 2.0

    TCS 105 7 98 2 97 3 0.2 0.5

    a 4-NP: 4-nonylphenol; BPA: bisphenol-A; TCS: triclosan.b Mean (ng/mL)standarddeviation (n =5, replicate samplestakenat thesametime).c

    LOD: limit of detection; LOQ: limit of quantitation.

    Table 3

    Concentrations of 4-NP, BPA and TCS in bottled water.

    Samples Compounds (ng/L)c

    4-NP BPA TCS

    S1 129 3 a 55.4 4.9 9.7 2.6

    S2 127 30 55.3 6.5 8.7 2.0

    S3 145 8 44.7 4.5 7.8 0.5

    S4 126 16 ND b ND

    S5 127 7 ND ND

    S6 111 14 ND ND

    S7 108 6 ND 0.6 0.1

    S8 122 12 22.8 1.7 1.6 0.1

    S9 130 2 129 97 2.1 0.8

    S10 111 24 78.5 7.1 2.1 0.2

    S11 148 43 155 40 2.6 0.1

    S12 236 29 324 47 3.6 0.4

    S13 219 6 56.2 17.6 3.4 0.2

    S14 298 53 285 18 3.2 0.0

    S15 217 16 52.0 18.3 3.6 0.1

    S16 210 47 17.6 0.7 1.9 0.0

    S17 186 35 45.2 47 2.9 1.3

    S18 163 21 18.0 2.0 2.2 0.2

    S19 271 63 23.4 4.6 2.2 0.1

    S20 181 3 19.3 0.2 2.5 0.2

    S21 204 5 19.0 0.4 2.5 0.2

    Min 108 17.6 0.6

    Max 298 285 9.7Median 170 82.4 3.5

    a Mean(ng/mL) standard deviation (n =3, replicate samplestakenat thesame time).b ND: not detected.c 4-NP: 4-nonylphenol; BPA: bisphenol-A; TCS: triclosan.

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    study wassimilar to theresults ofShao et al.(2005). BPAwas detected

    in 17 out of 21 bottled water samples in this study, while no BPA was

    detected in the previous study (Shao et al., 2005). Toyo'oka and

    Oshige (2000)reported the presence of 4-NP in mineral water from

    poly(ethylene terephthalate) (PET) bottles in concentrations ranging

    from 19 to 78 ng/L. Bottled water is usually sold in plastic containers,normally PET and high-density polyethylene (HDPE) as well as poly

    (vinyl chloride) (PVC). 4-NP could leach out from HDPE and PVC

    containers (Loyo-Rosales et al., 2004). BPA could be released into the

    water from polycarbonate (PC) drinking bottles at room temperature

    (Le et al., 2008). However, it is not clear whether the BPA detected in

    this study came from the drinking bottles or the water itself, or both.

    Estrogenicity in bottled mineral water has been reported in Germany,

    ranging from 2 to 40 ng/L EEQ (estradiol equivalent) (Wagner and

    Oehlmann, 2009), suggesting the presence of estrogenic compounds

    in the bottled water.

    Compared to the U.S.A. drinking water survey data by Benotti et al.

    (2009), the concentrations of BPA and TCS in tap water were similar

    while the levels of 4-NP were 10 times higher than that in their study.

    BPA was also detected at 160 ng/L in Brazilian drinking water, whichwasattributed to a large input of raw sewage into surface water (Sodr

    et al., 2009). On average, the concentration of 4-NP in winter samples of

    tap water was higher than in summer, while BPA and TCS were on the

    contrary. Variations in concentrations of the three compounds may be

    related to source water quality and treatment. All three compounds

    have been found in the source water of these six drinking water

    supplies, ranging between 288890 ng/L for 4-NP, 2.21030 ng/L for

    BPA and 0.6347 ng/L for TCS (Zhao et al., 2009). It suggests that the

    source water in some sections has been heavily polluted. In order to

    improve the quality of drinking water in Guangzhou, it is essential that

    control measures be applied to reduce the levels of these estrogenic

    compounds in source water.

    BPA is widely used as the monomer for the production of

    polycarbonate (PC) bottles. Previous reports show that BPA can

    leach out from PC containers (Biles et al., 1997; Sajiki and Yonekubo,

    2004; Wong et al., 2005; Le et al., 2008). The present study conrmed

    the continuous release of BPA from PC baby bottles under normal use

    conditions. High temperature (100 C) was found to greatly increase

    the release rate of BPA from the baby bottles. In fact, it is reported thatdishwashing, boiling and brushing could lead to polymer degradation

    (Brede et al., 2003), thus increasing the migration rate of BPA from

    baby bottles.

    The daily intake of 4-NP, BPA and TCS could be estimated by using

    the quantity of consumed drinking water according to the U.S. EPA:

    2 L per day for adults (60 kg body weight) and 1 L per day for infants

    (10 kg body weight) (U.S. EPA, 2006). The estimation was performed

    under two conditions (one using the average value of bottled water

    and tap water respectively for adults, and the other using the average

    value of tap water and the average concentration detected in the baby

    bottles at 40 C within 24 h for infants). From Table 7, if the entire

    water intake came from bottled water, an adult would ingest 340 ng/

    day of 4-NP, 165 ng/dayof BPA and 7 ng/day of TCS.If it camefromtap

    water, an adult would consume 1410 ng/day of 4-NP, 148 ng/day ofBPA and 10 ng/day of TCS,and an infant would ingest 705 ng/day of 4-

    Table 6

    Migration of bisphenol A from baby bottles at different times under normal use conditions.

    Brand Day 1 Day 3 Day 5 Day 7

    24 C 40 C 24 C 40 C 24 C 40 C 24 C 40 C

    B1 ND b 13 7 1.9 3.2 27 3 ND 38 6 ND 35 18

    B2 117 30 a 206 51 44 40 52 14 11 8 79 17 27 17 74 26

    B3 267 100 987 181 84 16 237 17 33 22 254 42 51 29 161 48

    B4 ND 9 2 24 31 24 1 ND 51 5 ND 1 2

    a Mean (ng)standard deviation released in 240 mL baby bottles (n =3).b

    ND: not detected.

    Table 4

    Concentrations of 4-NP, BPA and TCS in tap water from six water supply plants.

    Plants Phenolic compounds (ng/L)d

    4-NP BPA TCS

    June December June December June December

    P1 327 29 a 406 25 42.5 0.6 14.7 1.2 14.1 1.2 ND

    P2 286 29 199 66 54.3 1.8 123 8.4 4.1 0.4 ND

    P3 886 13 1160 62 171 2 61.8 5.9 11.9 0.1 ND

    P4 196 13 1150 89 7.0 0.8 23.8 1.5 4.1 0.1 ND

    P5 1070 106 566 38 317 5 19.8 15.6 14.5 1.2 ND

    P6 241 25 186 13 2.3 1.6 ND b bLOQc ND

    Min 196 186 2.3 19.8 bLOQ ND

    Max 1073 199 317 123 14.5 ND

    Median 502 909 99.0 48.6 9.7 ND

    a Mean (ng/mL) standard deviation (n =3, replicate samples taken at the same time).b ND: not detected.c

    bLOQ: below the limit of quantitation.d 4-NP: 4-nonylphenol; BPA: bisphenol-A; TCS: triclosan.

    Table 5

    Migration of bisphenol A from baby bottles at different temperatures within 24 h.

    Brand Amount released at different temperatures (ng)

    24 C 40 C 100 C

    B1 ND 13 7 309 107

    B2 117 30 a 206 51 311 185

    B3 267 100 987 181 4500 1940

    B4 ND b 9 2 34 4

    a Mean (ng)standard deviation released in 240 mL baby bottles (n =3).b ND: not detected.

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    NP, 1340 ng/day ofBPA and 5 ng/day ofTCS.From the results, it can be

    concluded that different types of water showed large variations of 4-

    NP consumption for adults.

    Daily intakes of 4-NP, BPA and TCS through consuming only tap

    water and mineral water varied between adults and infants. And the

    most concern according to this study is that the daily BPA intake for

    infants was3 times that for adults while infants were more vulnerable

    to these toxic substances. However, the daily intake values of 4-NP,

    BPA and TCS are much lower than their tolerable daily intake (TDI)

    values, which are 5g/kg body weight for NP (Nielsen et al., 2000),

    50g/kg body weight for BPA (Tsai, 2006) and 50 mg/kg body weightfor TCS (Dayan, 2007). The exposure anticipated from drinking water

    is just one of the many sources of EDC contamination; other sources

    such as food should be included in order to have a proper risk

    assessment for the three compounds. We also need to bear in mind

    that health risk assessment with a single compound may not fully

    reect the effects of exposures to EDC mixture in the real

    environment.

    5. Conclusion

    This study demonstrated that 4-NP, BPA and TCS were ubiquitous

    in drinking water including tap water, mineral water and pure

    drinking water. BPA can be released into the water from PC baby

    bottles at room temperature, 40 C and 100 C. Daily intake of 4-NP,BPA and TCS through drinking tap water is 1410 ng/day, 148 ng/day

    and 10 ng/day, respectively for adults, and 705 ng/day, 1340 ng/day,

    and 5 ng/day, respectively for infants. Most disturbingly, the daily

    intake of BPA for infants is nearly 10 times that for adults. However,

    based on this study, exposure to these three compounds from

    drinking water poses little risk to human health. But further research

    is needed to consider mixture effects and combined ingestion routes

    including food and water in order to make a more realistic human

    health risk assessment of daily intake of 4-NP, BPA and TCS.

    Acknowledgments

    The authors would like to acknowledge thenancial support from the

    National NaturalScience Foundationof China (NSFC40688001, 40771180and 40821003) and from the Guangdong Provincial Natural Science

    Foundation (8251064004000001). This is the contribution No. 1187 from

    GIGCAS.

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    Table 7

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    Bottled water Tap water Tap water (baby bottle at 40 C)

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