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Occurrence, distribution and fate of organic UV filters in coral communities Mirabelle M.P. Tsui, James C.W. Lam, Tsz Yan Ng, Put O. Ang, Margaret B. Murphy, and Paul Kwan-Sing Lam Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.6b05211 • Publication Date (Web): 29 Mar 2017 Downloaded from http://pubs.acs.org on April 1, 2017
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Occurrence, distribution and fate of organic UV filters in
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coral communities
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Mirabelle M.P. Tsui1, James C.W. Lam1,2*, T.Y. Ng3, P.O. Ang3, Margaret B. Murphy1,4,
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Paul K.S. Lam1,4
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and Human Health, Shenzhen Key Laboratory for Sustainable Use of Marine
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Biodiversity, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong
State Key Laboratory in Marine Pollution (SKLMP), Research Centre for the Oceans
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SAR, China
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Hong of Kong, Hong Kong SAR, China
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3
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Hong Kong, Shatin, N.T. Hong Kong SAR, China
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Avenue, Kowloon, Hong Kong SAR, China
Department of Science and Environmental Studies, The Education University of
Marine Science Laboratory, School of Life Sciences, The Chinese University of
Department of Biology and Chemistry, City University of Hong Kong, Tat Chee
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Corresponding Author
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* e-mail:
[email protected];
[email protected];
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Phone: +852 2948 8537, Fax: +852 2948 7676
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Keywords
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Organic ultraviolet filters, Coral, Metabolism, Bioaccumulation, Risk assessment
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Abstract
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Organic ultraviolet (UV) filters are widely used in personal care products and occur
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ubiquitously in the aquatic environment. In this study, concentrations of seven
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commonly used organic UV filters were determined in seawater, sediment and five
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coral species collected from the eastern Pearl River Estuary of South China Sea. Five
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compounds, benzophenone-1, -3 and -8 (BP-1, -3 and -8), octocrylene (OC) and octyl
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dimethyl-p-aminobenzoic acid (ODPABA), were detected in the coral tissues with the
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highest detection frequencies (>65%) and concentrations (31.8 ± 8.6 and 24.7 ± 10.6
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ng/g ww, respectively) found for BP-3 and BP-8. Significantly higher concentrations
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of BP-3 were observed in coral tissues in the wet season, indicating that higher inputs
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of sunscreen agents could be attributed to the increased coastal recreational activities.
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Accumulation of UV filters was only observed in soft coral tissues with
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bioaccumulation factors (log10-values) ranging from 2.21 to 3.01. The results of a
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preliminary risk assessment indicated that over 20% of coral samples from the study
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sites contained BP-3 concentrations exceeding the threshold values for causing larval
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deformities and mortality in the worst-case scenario. Higher probabilities of negative
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impacts of BP-3 on coral communities are predicted to occur in wet season.
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1. Introduction
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Human exposure to harmful ultraviolet (UV) radiation has increasing attention in
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recent decades due to increasing rates of skin cancers
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common ingredients of various types of personal care products (PCPs) such as
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sunscreens, lotions, and cosmetic products, for protecting human skin from sunburns,
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premature skin aging and skin cancer by absorbing UVA (315-400 nm) and UVB
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(280-315 nm). Apart from addition to PCPs, these chemical substances are also added
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to textiles, household products, plastics and paints to protect polymers and pigments
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against photodegradation and to prevent discoloring 3.
1,2
; organic UV filters are
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Organic UV filters can enter the aquatic environment (i) indirectly from wastewater
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treatment plants (WWTPs) after entering sewage systems following bathing or from
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industrial discharge and (ii) directly from recreational activities 4. The extensive
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application of organic UV filters has raised concerns about their potential
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environmental impact as they are pseudo-persistent in the environment and have
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shown adverse effects in aquatic organisms. They have been detected ubiquitously in
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various environmental matrices such as surface water 5, sediment 6 and soil 7. Owing
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to their lipophilicity (log Kow > 3), they show bioaccumulative potential and have
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been detected in aquatic organisms at low (e.g. mussels) 8 to high trophic levels (e.g.
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fishes and dolphins)
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organisms after exposure to organic UV filters, such as causing immobilization in
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Daphnia
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13,14
9,10
. Recent studies have reported adverse effects in aquatic
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, affecting reproduction in fish
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, affecting development in coral larvae
, and inducing coral bleaching 15.
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Coral reefs are one of the most biologically productive ecosystems on Earth and
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provide essential living habitat for countless marine organisms. However, reef
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ecosystems are under threat by global climate change, overfishing, coastal
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development, tourism, and water pollution 16,17. A previous report indicated that 88%
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of Southeast Asian coral reefs are at risk due to anthropogenic activities
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recent report has been predicted that coral bleaching and mortality would increase in
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magnitude and frequency over the next decades with the synergistic effects of ocean
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acidification and increasing in ocean temperature
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popularity of recreational activities in coral reefs, including swimming, snorkeling
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and scuba diving, brings an additional dimension of anthropogenic threat to coral
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reefs through the extensive use of PCPs that contain organic UV filters by visitors
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15,20
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; while a
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. Moreover, the increase in
.
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Hong Kong, situated on the west side of the Pearl River Delta in South China, is a
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highly urbanized area, whose marine environment is influenced by different emerging
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contaminants through various types of wastes and wastewater discharges from local
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WWTPs and the Pearl River Estuary (PRE) region, for examples, antibiotics 21, UV
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filters 22, halogenated flame retardants
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also notable marine biodiversity in the region; a recent survey indicated that the South
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China Sea hosts more than 570 known coral species, a richness that is comparable to
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the Coral Triangle
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genera and 12 families in Hong Kong, mainly found in eastern and southern waters 27.
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Previous studies have demonstrated the widespread occurrence (detection frequencies
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> 80%) of organic UV filters such as benzophenone-3 (BP-3), ethylhexyl
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methoxycinnamate (EHMC) and octocrylene (OC) in wastewater, sediment and
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surface water near coral habitats from Hong Kong
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and perfluoroalkyl substances
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. There is
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.There are 84 species of reef-building corals representing 28
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discharge due to incomplete removal by conventional treatments and recreational
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activities were reported as the major sources of contamination of these compounds in
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local waters. In addition, it was reported that exposure to the high concentrations of
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these compounds measured in recreational marine water samples near snorkeling
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hotspots in Hong Kong might result in adverse effects in corals
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preliminary risk assessment was only conducted by using surface water data and the
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bioaccumulative potential or bioconcentration factors of organic UV filters in few
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freshwater species were only reported in limited studies
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conventional organic pollutants (e.g. polycyclic aromatic hydrocarbons (PAHs)
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organochlorine pesticide
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distribution and fate of organic UV filters in coral and their associated aquatic
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environment (i.e. the ambient water and sediment) have not been reported and thus
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the potential adverse effects of these compounds might pose to these ecologically
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important coral ecosystems remain unknown. In order to investigate the effect of
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exposure of UV filters in corals, the objectives of this study therefore are (1) to
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determine the occurrence and distribution of seven commonly used organic UV filters,
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4-methylbenzylidene
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benzophenone-8 (BP-8), EHMC, OC and octyl dimethyl-p-aminobenzoic acid
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(ODPADA) in the ambient seawater column, associated sediment and coral samples
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of five species—Platygyra acuta, Porites sp., Pavona decussate, Acropora valida,
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and Favites abdita—collected from the eastern PRE (Hong Kong); (2) to study the
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tissue distribution and bioaccumulative potential, and (3) to conduct a preliminary
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environmental risk assessment for these ecologically important marine species. This
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study has provided information of occurrence of organic UV filters in water column,
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sediment and coral specimens for advancing our understanding of partitioning
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. However, the
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. Unlike other 32
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and polychlorinated biphenyls (PCBs) 34), the occurrence,
camphor
(4-MBC),
benzophenone-1
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BP-3,
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behavior of these compounds in coral ecosystems.
To our knowledge, this is the first
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report of the bioaccumulation factor (BAF) values of organic UV filters in the coral
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communities.
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2. Materials and methods
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2.1. Chemicals and solvents
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Standards for BP-3 (purity: 99.9%), BP-8 (99.9%), EHMC (99.2%), OC (98.9%) and
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ODPABA (99.2%) were obtained from United States Pharmacopeia Reference
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Standards (Rockville, MD, United States). 4-MBC (98.5%), BP-1 (99%) and
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ethylenediaminetetraacetic acid disodium salt dihydrate (Na2EDTA) were obtained
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from Sigma–Aldrich (St. Louis, MO, USA). Isotope-labeled
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purchased from Cambridge Isotope Laboratories Inc. (Andover, MA, USA). Detailed
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physicochemical characteristics of the targeted UV filters are shown in Table S1.
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Individual solutions of each analyte were prepared in pure methanol. Mixed standard
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solutions were prepared at 10 µg/mL in methanol and subsequently diluted as
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necessary. All standard solutions were stored in amber glass bottles at −20 °C to avoid
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photodegradation. Solvents including Milli-Q water (Millipore, Bedford, MA, USA),
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HPLC-grade methanol, HPLC-grade ethyl acetate (Merck, Darmstadt, Germany),
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pesticide-grade n-hexane and acetone (ACS, TX, USA) were utilized. Bond Elut C18
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(500 mg, 6 mL) cartridges (Agilent Technologies, Hong Kong) were used for sample
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extraction and purification.
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C-BP-3 (99%) was
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2.2. Sampling in coral habitats
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Coral samples (n=62) and corresponding ambient samples (i.e. water column, n=14;
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sediment, n=14) were collected from four locations (Ung Kong, Wu Pai, Sharp Island
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and Sung Kong) in Hong Kong in both the wet (August 2015) and dry (April 2015)
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seasons by scuba divers (Table S2). Coral specimens were collected from Hong Kong
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waters following the conditions stipulated by the Agriculture, Fisheries and
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Conservation Department of the Hong Kong government. To minimize possible
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impacts to local coral communities, only a small fragment (approximately 2 × 2 cm in
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size) was carefully removed from intact pieces of coral. Resampling of the same
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colony was avoided during the study period to eliminate or minimize any possible
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stress- or injury-induced response which may affect coral health, including their
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ability to reproduce. It should be noted that coral specimens of the same species were
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not be collected at all locations and in both seasons due to the coral availability at
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each sampling site. A permit under the Convention on International Trade in
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Endangered Species of Wild Fauna and Flora (CITES) was not required in this study
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as no import or export of these specimens occurred.
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Detailed information on sampling locations is shown in Figure S1. Sai Kung is
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located in the eastern marine waters of Hong Kong and features generally good water
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quality
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activities including snorkeling, scuba diving and swimming are frequently conducted
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in these areas, especially in the summer. Ung Kong and Sharp Island are both diving
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hotspots in Sai Kung. These two locations were characterized by over 70% coral
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coverage in a 2014 survey 35. Wu Pai is located in the northeast of the territory at Mirs
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Bay, in which the aquatic environment is controlled by a jointly formulated water
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quality control strategy by Hong Kong and the city of Shenzhen in mainland China.
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The 2014 survey recorded over 65% coral coverage in this area
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Island is part of the Po Toi Islands located in southeastern Hong Kong waters. Diving
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with a diversity of marine life such as corals. Therefore, recreational
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. Sung Kong
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activities are conducted less frequently at Sung Kong than at the other three study
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sties due to strong currents and low (
