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Marine Pollution Bulletin 60 (2010) 1376–1382

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Marine Pollution Bulletin 60 (2010) 1376–1382 Marine Pollution Bulletin 60 (2010) 1376–1382 Contents lists available at ScienceDirect Marine Pollution Bulletin journal homepage: www.elsevier.com/locate/marpolbul Baseline Caffeine and agricultural pesticide concentrations in surface water and groundwater on the north shore of Kauai (Hawaii, USA) Karen L. Knee a,b,*, Richard Gossett c, Alexandria B. Boehm d, Adina Paytan b a Department of Geological and Environmental Sciences, Stanford University, Stanford, CA 94305, USA b Institute of Marine Sciences, University of California, Santa Cruz, 1156 High St., Santa Cruz, CA 95064, USA c Institute for Integrated Research in Materials, Environments, and Society, 1250 Bellflower Blvd., California State University, Long Beach, Long Beach, CA 90840, USA d Environmental and Water Studies, Department of Civil and Environmental Engineering, Stanford University, Stanford, CA 94305, USA article info abstract Keywords: Caffeine has been associated with wastewater pollution in temperate and subtropical locations, but envi- Caffeine ronmental caffeine concentrations in tropical locations have not been reported. The objectives of this Hawaii study were to measure caffeine and agricultural pesticide (carbaryl, metalaxyl, and metribuzin) concen- Metribuzin trations in environmental waters on the tropical north shore of Kauai (Hawaii, USA) and assess whether Wastewater patterns in caffeine concentration were consistent with a wastewater caffeine source. Groundwater, river, Tropical stream and coastal ocean samples were collected in August 2006 and February 2007. Caffeine was Coastal detected in all August 2006 samples and in 33% of February 2007 samples at concentrations up to 88 ng LÀ1. Metribuzin was detected in five samples collected in February 2007. Carbaryl and metalaxyl were not detected in any sample. Caffeine was not detected in offshore ocean samples or river samples upstream of human development. A positive correlation between caffeine and enterococci suggested a possible wastewater caffeine source. Ó 2010 Elsevier Ltd. All rights reserved. Caffeine (C8H10N4O2), a xanthine alkaloid compound and cen- water quality is essential for the health of the north shore’s coral tral nervous system stimulant, is the most widely used psychoac- reefs, human swimmers, and the tourism-based economy. In tive drug in the world. About 90% of North American adults 2007, the most recent year for which complete data were available, consume caffeine daily, mainly in the form of coffee, tea, or caffe- over 1.3 million tourists visited Kauai, with 70% spending time at inated soft drinks (Lovett, 2005). Approximately 3% of a person’s the beach and 37% snorkeling or SCUBA diving (State of Hawaii, caffeine intake is excreted in the urine (Tang-Liu et al., 1983). Thus, 2007). caffeine can enter the wastewater stream either in urine or when Intermittently high levels of enterococci, the fecal indicator bac- caffeine-containing products, such as beverages or pharmaceuti- teria used to set water quality standards in the United States and cals, are disposed of through household plumbing and sewer sys- the state of Hawaii, have been detected in beach and river water tems (Seiler et al., 1999). Studies in the mainland United States on the north shore of Kauai since 2000 (Hanalei Watershed Hui, (Siegener and Chen, 2002; Peeler et al., 2006), Europe (Buerge unpublished data), raising concerns about sewage contamination. et al., 2003; Weigel et al., 2004) and Australia (Chen et al., 2002) Except for the Princeville community east of the Hanalei River have linked caffeine concentrations in ground and surface waters (Fig. 1), which has a wastewater treatment plant (WWTP), the to wastewater contamination and suggested that caffeine could north shore relies on septic systems and cesspools. Previous work be used as a wastewater tracer. However, to the best of our knowl- (Knee et al., 2008) suggested that fecal indicator bacteria enter edge, environmental caffeine concentrations in tropical regions beach water mainly via rivers and streams and not from ground- have not been reported. water discharge or contaminated sand. However, whether water- This study aimed to address that gap by measuring environ- borne enterococci originate from human sewage or the feces of mental caffeine concentrations on the north shore of Kauai wild or domestic animals remains unknown. Naturally occurring (Fig. 1), a tropical, relatively undeveloped area. Maintaining good enterococci bacteria have also been reported in Hawaiian (Hardina and Fujioka, 1991) and Guamanian (Fujioka et al., 1999) soils and streams, suggesting that they may not always be associated with * Corresponding author at: Department of Geological and Environmental Sci- fecal pollution in these, and likely other, tropical locations. ences, Stanford University, Stanford, CA 94305, USA. Tel.: +1 650 862 4739; fax: +1 Novel wastewater tracers, such as caffeine, may be useful for 650 723 7058. E-mail addresses: [email protected] (K.L. Knee), [email protected] (R. identifying fecal pollution in tropical settings where traditional Gossett), [email protected] (A.B. Boehm), [email protected] (A. Paytan). indicator bacteria grow naturally. Caffeine may also be a pollutant 0025-326X/$ - see front matter Ó 2010 Elsevier Ltd. All rights reserved. doi:10.1016/j.marpolbul.2010.04.019 K.L. Knee et al. / Marine Pollution Bulletin 60 (2010) 1376–1382 1377 Fig. 1. Map of sites where samples were collected. Adapted with permission from Knee et al. (2008). Bulls-eye symbols indicate coastal ocean sampling sites. Gray lines on the bottom panel indicate rivers and streams. Shading indicates land use (black for urban development; dark gray for agriculture; light gray for grasslands; and white for undeveloped land, including forests, wetlands, and barren land). Land use data are from National Oceanographic and Atmospheric Administration Coastal Services Center (www.csc.noaa.gov/crs/lca/hawaii.html). in its own right. A recent study (Pollack et al., 2009) suggested that 2007). However, no coral bleaching has been reported (Friedlander exposure to caffeine may exacerbate the effects of other environ- et al., 2008), and the north shore of Kauai is one of the few places in mental stressors on corals, making them more likely to undergo Hawaii where coral cover has actually increased over the past dec- bleaching. ade (Brown and Friedlander, 2007). Pesticides are another class of terrestrial pollutants that pose a Accordingly, the primary goal of this study was to provide a pre- threat to coral reefs and other coastal ecosystems. A previous study liminary survey of caffeine, carbaryl, metalaxyl, and metribuzin of the Hanalei River (Orazio et al., 2007; Fig. 1) found low water- concentrations in groundwater and surface water at various sites borne concentrations of the insecticide dieldrin; however, the on the north shore of Kauai. A secondary goal was to assess authors did not measure pesticide concentrations in groundwater whether the pattern of caffeine concentrations we observed was or coastal ocean water. In the present study, we tested for carbaryl, consistent with a wastewater source, a natural source, or a combi- metalaxyl, and metribuzin, three agricultural pesticides used in nation of the two. Hawaii (Brennan et al., 1992). These three pesticides were selected During two sampling periods in August 2006 and February for the following reasons: (1) they have octanol-water partition 2007, a total of 61 groundwater and surface water samples were coefficients indicating solubility in water, (2) publications and gov- collected from five sites along the north shore of the island of ernment reports (Kasimani, 1988; Brennan et al., 1992; Miles et al., Kauai, including Hàena, Hanalei Bay, and Hono Iki (Fig. 1, Table 1). 1992; Deputy and Hara, 2000) suggested that they might be used The population densities and land use patterns in the vicinity of on the north shore of Kauai, and (3) they could be analyzed concur- each site are reported in a previous paper (Knee et al., 2008). Four rently with caffeine, which was the main focus of the study. supplementary samples (two from the Hanalei River upstream of In addition, the three pesticides we surveyed can negatively af- all human development and two from the offshore ocean outside fect aquatic organisms. Carbaryl, an insecticide used on farms and of Hanalei Bay) were collected in March 2008. lawns, can inhibit coral larval metamorphosis (Markey et al., 2007). Groundwater and surface water samples were collected at each Metalaxyl, a fungicide, is toxic to algae and zooplankton (Kungolos site (Table 1). Groundwater samples included water flowing from et al., 2009), and metribuzin, an herbicide, can harm corals’ symbi- coastal springs and pumped from temporary wells installed in otic dinoflagellate algae, leading to impaired photosynthesis and the beach face. Temporary wells consisted of either a hand-dug bleaching (Jones, 2005). Coral disease, perhaps related to stress pit with a screened bucket inserted in it or an augured hole with from sedimentation, has been documented in Hanalei Bay (Aeby, a screened PVC pipe; these wells accessed unconfined groundwater 1378 K.L. Knee et al. / Marine Pollution Bulletin 60 (2010) 1376–1382 Table 1 Analytes were extracted into dichloromethane using liquid–li- Caffeine detection and average concentration. Concentrations are either the value of quid extraction. All glassware used for extraction was soap- the single sample (if n = 1) or the group mean value (if n > 1). When some samples
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