Elsevier

Chemosphere

Volume 62, Issue 6, February 2006, Pages 867-873
Chemosphere

A survey of polycyclic musks in selected household commodities from the United States

https://doi.org/10.1016/j.chemosphere.2005.10.006Get rights and content

Abstract

Occurrence of the polycyclic musks, 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta[g]-2-benzopyran (HHCB) and 7-acetyl-1,1,3,4,4,6-hexamethyl-1,2,3,4-tetrahydronapthalene (AHTN), in wastewater influent and effluent, as well as in surface waters, has been reported. HHCB and AHTN were also reported to occur in human and wildlife tissues. The major sources for HHCB and AHTN to wastewater are thought to be consumer products such as shampoos, deodorants, laundry detergents, and household surface cleaners. However, the levels of HHCB and AHTN in consumer products are not known. For evaluation of the sources of human and environmental exposures, characterization of levels of HHCB and AHTN in consumer products is needed. In this study, we measured concentrations of HHCB (Galaxolide®), AHTN (Tonalide®), and HHCB-lactone (Galaxolidone®) from a variety of consumer products, including perfumes, body lotions, and deodorants. Concentrations of HHCB, AHTN, and HHCB-lactone in consumer products ranged from <5 ng/g to over 4000 μg/g, <5 ng/g to 451 μg/g, and <5 ng/g to 217 μg/g, respectively. The highest concentrations were found in perfumes, body creams and lotions, and deodorants. The results suggest that a wide variety of source materials exist for HHCB and AHTN, and that these materials are used on a daily basis.

Introduction

Since the 1950s, there has been widespread use of polycyclic musks as fragrances in cosmetics and detergents (Dsikowitzky et al., 2002). Polycyclic musks are considered desirable because of their pleasant odor, inexpensive synthesis (as compared to other synthetic musk compounds), and their affinity to bind to fabrics (Sommer and Juhl, 2004). The two main polycyclic musks used in consumer products are 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta[g]-2-benzopyran (HHCB) and 7-acetyl-1,1,3,4,4,6-hexamethyl-1,2,3,4-tetrahydronapthalene (AHTN). Both substances are included on the OSPAR Commission (Oslo and Paris Commission) list of chemicals for priority action (OSPAR, 2000). In 1996, the worldwide production of polycyclic musks, 90–95% of which were HHCB and AHTN, was 5600 tons (Rimkus, 1999). In the United States, HHCB is listed by the US Environmental Protection Agency (EPA) as a high production-volume chemical, a rating which suggests that the production is more than 4500 tons per year, for uses that are reportable under the Toxic Substances Control Act (USEPA, 2003).

Occurrence of HHCB and AHTN in human adipose tissues from Germany, Switzerland, and the United States has been reported (Müller et al., 1996, Rimkus and Wolf, 1996, Kannan et al., 2005). Recently, HHCB and AHTN have been shown to accumulate in the tissues of marine mammals and fish collected from Japanese and US coastal waters (Kannan et al., 2005, Nakata, 2005). Several studies have reported the widespread occurrence of HHCB and AHTN in surface water, sediment, and biota collected in Western European countries (Draisci et al., 1998, Fromme et al., 1999, Gatermann et al., 1999, Dsikowitzky et al., 2002, Bester, 2004). The characterization and assessment of sources of human and environmental exposures to polycyclic musks are subjects of current interest (Cadby et al., 2002, Salvito et al., 2004).

A variety of household products, such as cosmetics, perfumes, air fresheners, soaps and detergents and cleaning products (shampoos, fabric softeners), contain these polycyclic musks because of the musky scent that they impart (Sommer and Juhl, 2004). As a result, consumers may be exposed to varying doses of HHCB and AHTN, depending on the usage of certain household commodities. In household commodities, complex perfume-mixtures containing polycyclic musks purchased as such from the fragrance producers are used at varying ratios. Therefore, actual concentrations of HHCB and AHTN in various consumer products will differ as a function of the formulations (HERA, 2004). Until now, no surveys have reported the levels of HHCB and AHTN in consumer products from the United States. Determination of levels of HHCB and AHTN in consumer products is important to evaluate and to characterize potential sources of human and environmental exposures.

Daily use of certain household products also results in the release of polycyclic musks via rinsing or washing down the drain, leading to discharges into the sewage system (Bester, 2005). It is the down-the-drain route of exposure for fragrance materials that is considered to be the primary environmental pathway (Salvito et al., 2004). Recent studies from Europe and the United States have reported the widespread occurrence of HHCB and AHTN in wastewater influent and effluent (Gatermann et al., 1999, Herren and Berset, 2000, Simonich et al., 2002, Ricking et al., 2003, Bester, 2005). The metabolite of HHCB, HHCB-lactone, has also been detected in wastewater in European countries. Concentrations of HHCB and AHTN in influent and effluent from wastewater treatment plants from various countries are shown in Table 1.

The purpose of this study was to determine concentrations of HHCB, AHTN, and HHCB-lactone in selected consumer products purchased in retail stores in the United States to enable an assessment of the sources of exposure to humans.

Section snippets

Samples

Sixty household commodities, including perfumes, lotions, hair care products, and household cleaners, were purchased from retail stores in Albany, New York. The household commodities were grouped as: perfumes, including body splash, oil, eau de toilette, and body mist (n = 7); body lotions, including moisturizing lotion and body cream (n = 7); deodorants/antiperspirants (n = 4); shower gels/soaps/shaving creams (n = 14); shampoos/conditioners/hair products, including hair gel and hair cream (n = 12); and

Results and discussion

Sixty household commodities were measured for the polycyclic musks HHCB and AHTN, along with HHCB-lactone, a metabolite of HHCB. Samples were grouped into six categories, depending on the purpose of application, as perfumes, body lotions and creams, deodorants and antiperspirants, shower gels and shaving creams, hair products, and household sanitation products. HHCB was detected in 72% of the samples analyzed, AHTN was detected in 32% of the samples, and HHCB-lactone was detected in 40% of the

Conclusions

The household products measured in this study contained varying concentrations of HHCB, AHTN, and HHCB-lactone. Few data have been published on the concentrations of polycyclic musks in consumer products; thus, to our knowledge, this is the first study on the concentrations of polycyclic musks in such household products. Overall, 77% of the household products analyzed in this study contained measurable levels of at least one of the three polycyclic musks assayed. The measured concentrations

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