Polycyclic Musks in the Air and Water of the Lower Great Lakes: Spatial Distribution and Volatilization from Surface Waters

Abstract

Polycyclic musks (PCMs) are synthetic fragrance compounds used in personal care products and household cleaners. Previous studies have indicated that PCMs are introduced to aquatic environments via wastewater and river discharge. Polyethylene passive samplers (PEs) were deployed in air and water during winter 2011 and summer 2012 to investigate the role of population centers as sources of these contaminants to the Great Lakes and determine whether the lakes were acting as sources of PCMs via volatilization. Average gaseous ΣPCM ranged from below detection limits (<DL) to 3.2 ng/m on the western shoreline of Lake Erie in Toledo. Average dissolved ΣPCM ranged from <DL to 2.6 ng/L on the southern shore of Lake Ontario near the mouth of the Oswego River. Significant correlations were observed between population density and ΣPCM in both air and water, with strongest correlations within a 25 and 40 km radius, respectively. At sites where HHCB was detected it was generally volatilizing, while the direction of AHTN air-water exchange was variable. Volatilization fluxes of HHCB ranged from 11 ± 6 to 341 ± 127 ng/m/day, while air-water exchange fluxes of AHTN ranged from -3 ± 2 to 28 ± 10 ng/m/day. Extrapolation of average air-water exchange flux values over the surface area of the lakes' coastal boundary zone suggested volatilization may be responsible for the loss of 64-213 kg/year of dissolved ΣPCM from the lakes.

Urban sources of synthetic musk compounds to the environment

“…69 In general, the median S 6 PCMs was $3 times higher at the 3 most urban sites, which were located at 0 km, 1 km, and 5 km from the city centre, than at the 3 most rural sites, which were located 40 km, 60 km and 80 km from the city centre. Our results are consistent with those of McDonough et al 41 who found significant correlations between population density and S 5 PCMs (ADBI, AHMI, ATII, HHCB, AHTN) in both air and water. We hypothesize that PCM sources supporting this gradient are the collective emissions from indoor air via building ventilation and from WWTPs during the treatment process.…”

“…Most studies on SMCs have focused on NMs and PCMs with fewer conducted on MCMs. 1,30,31 NMs and PCMs have been reported in indoor dust, 1,[32][33][34] indoor air, 32,35,36 outdoor air, [37][38][39][40][41][42] biota; 43-48 surface waters; 37,41,49-51 sea water, 37 sediments, 52 wastewater treatment plants (WWTPs); [53][54][55] drinking water, 56 human adipose tissue, 45,57,58 breast milk, 31,[59][60][61] and serum. 59,62 The potential for SMCs to undergo long-range transport is debatable.…”

“…sum of HHCB and AHTN) to Lake Ontario were from waste water treatment plant (WWTP) effluent which accounted for 83% of total loadings, with minor contributions from atmospheric deposition (10%) and tributary discharge into the lake (7%). McDonough et al 41 reported that in Lake Ontario and Lake Erie, HHCB underwent net volatilization from water to air but the ux was variable for AHTN. The authors suggested that volatilization could be responsible for the loss of 64 to 213 kg PCMs per year from the lakes.…”

Field‐testing polyethylene passive samplers for the detection of neutral polyfluorinated alkyl substances in air and water

“…Three deuterated polycyclic aromatic hydrocarbons (PAHs; fluorene-d 10 , pyrene-d 10 , and benzo[a] pyrene-d 12 ) were used as PRCs; average PRC losses were 97% for fluorene-d 10 , 61% for pyrene-d 10 , and 2% for benzo[a]pyrened 12 . Sampling rates (R s ) were calculated as detailed in previous studies (McDonough et al 2016a(McDonough et al , 2016b. In the WWTP deployments performed here, R s averaged 28.1 AE 4.4 L/d.…”

“…The ratio of target compound concentrations (at equilibrium) in the same passive sampler matrix between water and air was used to derive water-to-air gradients (chemical activity gradients), and corresponding gaseous air-water exchange fluxes (Liu et al 2016;McDonough et al 2016aMcDonough et al , 2016b. Because ratios were based on PFASs that had equilibrated (day 28 for WWTP effluents, days 16 and 32 for air polyethylene), the ratios were not influenced by R s or K PE values.…”