Article pubs.acs.org/est
Paraben Concentrations in Maternal Urine and Breast Milk and Its Association with Personal Care Product Use Mandy Fisher,*,† Susan MacPherson,† Joseph M. Braun,‡ Russ Hauser,§ Mark Walker,∥ Mark Feeley,⊥ Ranjeeta Mallick,∥ René Bérubé,# and Tye E. Arbuckle† †
Healthy Environments and Consumer Safety Branch, Health Canada, Ottawa, ON, Canada Department of Epidemiology, Brown University, Providence, Rhode Island 02912, United States § Harvard University School of Public Health, Boston, Massachusetts, United States ∥ The Ottawa Hospital Research Institute, Ottawa, ON, Canada ⊥ Health Products and Food Branch, Health Canada, Ottawa, ON, Canada # Institut National de Santé Publique du Québec, Québec, QC Canada ‡
S Supporting Information *
ABSTRACT: Parabens are broad-spectrum antimicrobial preservatives and fragrances used in a wide range of personal care products, pharmaceuticals, and food providing the opportunity for people to be exposed on a daily basis. In 2009−2010, 80 pregnant women from Ottawa Canada participated in the Plastics and Personal-Care Product Use in Pregnancy (P4) Study. A subset of women (n = 31) who provided multiple spot urine samples (n = 542) collected over two 24-h periods had their samples analyzed for methylparaben (MP), npropylparaben (PP), ethylparaben (EP), butylparaben (BP), isobutylparaben (IBP), and benzylparaben (BzP). These parabens were also measured in breast milk samples collected at approximately 3 months postpartum (n = 56 women). Women kept a diary of products that they used 24 h prior to and during the collection. All parabens measured in maternal urine had moderate to high reproducibility. Women who used lotions in the past 24 h had significantly higher geometric mean paraben concentrations (80−110%) in their urine than women who reported no use in the past 24 h. Women who used shampoo, conditioner, and cosmetics also showed 70−80% higher BP concentrations in their urine. Breast milk samples had >50% detection for MP, PP, and EP.
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INTRODUCTION
examining breast milk levels of parabens and use of personal care products have not been published. Parabens exhibit very weak estrogenic activity in vitro and in vivo.8 In some recent papers urinary paraben concentrations have been associated with oxidative stress in pregnant women9 and sperm DNA damage in men.7 However, the Cosmetic Ingredient Review (CIR)10 and the U.S. Food and Drug Administration (FDA)11 have concluded that there is no reason for consumers to be concerned about parabens at concentrations used in cosmetics (up to 0.4% for a single paraben or 0.8% for mixtures of parabens). The European Union Scientific Community on Consumer Safety (SCCS)12 considers MP and ethylparaben (EP) safe at the maximum authorized concentrations in cosmetics, whereas butylparaben and PP are safe in cosmetics as long as the sum of their individual concentrations does not exceed 0.19%. Based on current levels of use, cosmetics containing parabens do not pose a significant health
Parabens are broad-spectrum antimicrobial preservatives and fragrances used in a wide range of personal care products and pharmaceuticals, as well as in food and beverage processing leading to widespread exposure in the general population on a daily basis.1,2 In the US 2005−06 National Health And Nutrition Examination Survey (NHANES), methylparaben (MP) and n-propylparaben (PP) were detected in 99.1% and 92.7% of 2,548 urine samples, respectively, while ethyl (42.4%) and butyl (47%) parabens were less frequently detected.1 Parabens have also been measured in breast milk;3−5 however, to the best of our knowledge there are no published data on parabens in Canadian human milk. In the 2005−06 NHANES, female participants were three to four times more likely than male participants to have urinary concentrations of MP and PP above the 95th percentile.1 This may be due to the more frequent and intense use of personal care products among women. Indeed, use of lotions, cosmetics, hair gel, or cologne/perfume in the past 24 h has been shown to be associated with higher concentrations of urinary parabens among women.6,7 However, to our knowledge, studies © XXXX American Chemical Society
Received: August 24, 2016 Revised: November 22, 2016 Accepted: December 9, 2016
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DOI: 10.1021/acs.est.6b04302 Environ. Sci. Technol. XXXX, XXX, XXX−XXX
Article
Environmental Science & Technology risk to consumers.13 Health Canada plans to assess various parabens as part of the third phase of the Chemicals Management Plan over the next four years (2016−2020).14 Parabens have short half-lives and are rapidly excreted from the body. One study has reported that butylparaben concentrations peaked in urine within 8−12 h after topical application.15 Little is known about how levels of parabens vary over time due to day-to-day changes in exposure from personal product use, activity patterns, and other environmental or biological factors. In order to assess the potential risk associated with paraben exposure it is important to have valid and reliable measures of human exposure, understand the effects of time of day on observed urinary levels, and know whether measurement in one urine sample represents the individual’s exposure throughout a 24-h or longer period. In this study we measured parabens in maternal urine and breast milk to determine the extent to which women are exposed to parabens during pregnancy and 2−3 months postpartum, estimate intraindividual variability, and explore the association between the use of personal care products and paraben concentrations.
with ice packs in order to avoid degradation of the target chemicals.18 A research assistant from the Ottawa Hospital visited the participants’ home to collect the urine samples within 36 h of the women’s first sample. After collection each urine sample was homogenized in a vortex mixer for 5 s, aliquotted into 5 mL Simport containers within 36 h of collection, and stored in a −80 °C freezer. Breast Milk. A breast milk sample was collected at the woman’s home at the T5 visit 2−3 months after delivery (n = 56). The woman was asked to collect the breast milk either during the 24 h prior to the home visit or at the home visit. Women were provided with glass jars as well as a Medela breast pump. Women recorded the date and time of the sample collection, which breast they collected it from, the time since the last feed from that breast and the name of any creams, lotions, or cleansers used on their breast. The method of collection was also recorded (hand or manual expression, mechanical breast pump vs mechanical/electric breast pump). Field Blanks. A number of field blanks (5 for urine and 7 for breast milk) were used to assess the potential risk of biospecimen contamination during collection or processing of the urine and breast milk samples. Steril.O reagent grade deionized distilled water was used as the sampling medium. For the urine, each cooler bag provided to the women for her urine collection also contained a sealed field blank consisting of a urine collection container with approximately 50 mL of deionized water. For the breast milk field blanks, glass jars containing 50 mL of deionized water, appropriately labeled as “field blank”, were provided to the women prior to collection, along with the breast milk collection kit. No trace contamination was detected in any of the field blanks. Personal Care Product Use Information. At the same time as the urine collection, women were asked to complete a diary that asked them to record their activities, food consumption, and personal care product use throughout the day. For the T1A and T1B time points the diary was completed for a 48 h period starting 24 h prior to commencing urine collection and during the 24 h of urine collection. At the T5 study period, participants completed the diary 24 h prior to the urine and breast milk collection. Participants were asked to indicate the time of day and type of product used. The personal care product content of the diaries were manually categorized into the following 16 mutually exclusive categories: (1) Fragrance and Perfumed Products; (2) Deodorant and Antiperspirants; (3) General Make-up and Cosmetics; (4) Hair Styling Products; (5) Eye Make-up and Cosmetics; (6) Nail Polish and Remover; (7) Body Lotions and Creams; (8) Face Lotions and Creams; (9) Facial Soaps, Cleanser and Washes; (10) Baby Lotions, Soaps and other Baby Products; (11) Hand Soaps, Sanitizers and Soap not otherwise specified (NOS); (12) Body Soaps; (13) Shampoo; (14) Conditioner; (15) Toothpaste and Mouthwash; (16) Lip Products. For further details see Lang et al.19 Laboratory Analysis. Butylparaben (BP), methylparaben (MP), n-propylparaben (PP), ethylparaben (EP), isobutylparaben (IBP), and benzylparaben (BzP) were measured on only the participants (n = 31, n = 542 samples) who collected the 24 h serial spot urines on both a weekday (T1A) and weekend day (T1B) when they were less than 20 weeks pregnant. Breast milk was successfully collected from 56 participants at the postpartum visit (T5 study period) and analyzed for the same set of parabens.
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MATERIALS AND METHODS The Plastics and Personal-Care Product Use in Pregnancy (P4) Study was conducted between November 2009 and December 2010. The methods have been described in detail elsewhere.16,17 Briefly, 80 pregnant women were recruited from the Ottawa Hospital and asked to collect serial urine samples during early pregnancy. Eligibility criteria included the ability to consent and communicate in English or French, age 18 years or older, less than 20 weeks pregnant and planning on delivering at a local hospital. Exclusions included: women who had known chromosomal abnormalities or major malformations in the current pregnancy; women who have a history of medical complications, and women who are already participating in two or more research projects. Written consent was obtained and a copy of the signed consent form provided to the woman for her records. As part of the consent form, the participants agreed to have any leftover samples stored for future research directly related to environmental contaminants. On recruitment, women were asked to complete a short questionnaire that collected demographic, socio-economic, obstetrical history, smoking history, and current pregnancy information, as well as information on their occupation and potential sources of exposure to the chemicals of interest (such as the use of personal care products). The study had 5 separate data collection time points: T1A (week day) and T1B (weekend day) at
