Time trends of polycyclic aromatic hydrocarbon exposure in New York City from 2001 to 2012: assessed by repeat air and urine samples

Abstract

Background: Exposure to air pollutants including polycyclic aromatic hydrocarbons (PAH), and specifically pyrene from combustion of fuel oil, coal, traffic and indoor sources, has been associated with adverse respiratory health outcomes. However, time trends of airborne PAH and metabolite levels detected via repeat measures over time have not yet been characterized. We hypothesized that PAH levels, measured repeatedly from residential indoor and outdoor monitors, and children׳s urinary concentrations of PAH metabolites, would decrease following policy interventions to reduce traffic-related air pollution.

Methods: Indoor PAH (particle- and gas-phase) were collected for two weeks prenatally (n=98), at age 5/6 years (n=397) and age 9/10 years (n=198) since 2001 and at all three age-points (n=27). Other traffic-related air pollutants (black carbon and PM2.5) were monitored indoors simultaneous with PAH monitoring at ages 5/6 (n=403) and 9/10 (n=257) between 2005 and 2012. One third of the homes were selected across seasons for outdoor PAH, BC and PM2.5 sampling. Using the same sampling method, ambient PAH, BC and PM2.5 also were monitored every two weeks at a central site between 2007 and 2012. PAH were analyzed as semivolatile PAH (e.g., pyrene; MW 178-206) (∑8PAH(semivolatile): Including pyrene (PYR), phenanthrene (PHEN), 1-methylphenanthrene (1-MEPH), 2-methylphenanthrene (2-MEPH), 3-methylphenanthrene (3-MEPH), 9-methylphenanthrene (9-MEPH), 1,7-dimethylphenanthrene (1,7-DMEPH), and 3,6-dimethylphenanthrene (3,6-DMEPH)) and the sum of eight nonvolatile PAH (∑8PAH(nonvolatile): Including benzo[a]anthracene (BaA), chrysene/iso-chrysene (Chry), benzo[b]fluoranthene (BbFA), benzo[k]fluoranthene (BkFA), benzo[a]pyrene (BaP), indeno[1,2,3-c,d]pyrene (IP), dibenzo[a,h]anthracene (DahA), and benzo[g,h,i]perylene (BghiP); MW 228-278). A spot urine sample was collected from children at child ages 3, 5, 7 and 9 between 2001 and 2012 and analyzed for 10 PAH metabolites.

Results: Modest declines were detected in indoor BC and PM2.5 levels between 2005 and 2012 (Annual percent change [APC]=-2.08% [p=0.010] and -2.18% [p=0.059] for BC and PM2.5, respectively), while a trend of increasing pyrene levels was observed in indoor and outdoor samples, and at the central site during the comparable time periods (APC=4.81%, 3.77% and 7.90%, respectively; p<0.05 for all). No significant time trend was observed in indoor ∑8PAH(nonvolatile) levels between 2005 and 2012; however, significant opposite trends were detected when analyzed seasonally (APC=-8.06% [p<0.01], 3.87% [p<0.05] for nonheating and heating season, respectively). Similarly, heating season also affected the annual trends (2005-2012) of other air pollutants: the decreasing BC trend (in indoor/outdoor air) was observed only in the nonheating season, consistent with dominating traffic sources that decreased with time; the increasing pyrene trend was more apparent in the heating season. Outdoor PM2.5 levels persistently decreased over time across the seasons. With the analyses of data collected over a longer period of time (2001-2012), a decreasing trend was observed in pyrene (APC=-2.76%; p<0.01), mostly driven by measures from the nonheating season (APC=-3.54%; p<0.01). In contrast, levels of pyrene and naphthalene metabolites, 1-hydroxypyrene and 2-naphthol, increased from 2001 to 2012 (APC=6.29% and 7.90% for 1-hydroxypyrene and 2-naphthol, respectively; p<0.01 for both).

Conclusions: Multiple NYC legislative regulations targeting traffic-related air pollution may have led to decreases in ∑8PAH(nonvolatile) and BC, especially in the nonheating season. Despite the overall decrease in pyrene over the 2001-2012 periods, a rise in pyrene levels in recent years (2005-2012), that was particularly evident for measures collected during the heating season, and 2-naphthol, indicates the contribution of heating oil combustion and other indoor sources to airborne pyrene and urinary 2-naphthol.

Keywords: Heating oil combustion; Polycyclic aromatic hydrocarbons; Repeat exposure; Temporal variations; Trafficemission; Urinary metabolites.

Fig. 1. Pollutant data available in various ages of subjects (prenatal through age 9/10) and various sampling matrices

At each age including prenatally, subjects were enrolled over 4–7 years for air pollution and 5–9 years for urinary PAH metabolites. ^a9 PAH (8 nonvolatile PAH and one semivolatile pyrene) were measured. ^b16 PAH (8 nonvolatile and 8 semivolatile) were measured.

Fig. 2. Follow-up of children for (a) airborne residential indoor PAH monitoring and (b) urinary PAH metabolite data

I: one measure, II: two measures, III: three measures; IV: four measures; Only 27 children had indoor monitoring data at all three age-points and 179 children had urinary PAH metabolite data at all four time-points.

Fig. 3. Temporal trends of (a) pyrene and (b) Σ₈PAH_nonvolatile concentrations measured from the central site from 2007 to 2012, stratified by heating season

Annual arithmetic mean concentrations of central site PAH levels with 95% confidence interval are presented by heating season; Linear regression modeling was used to test trends over time; The percent change in PAH concentration per year was calculated by 100*[exp(log_β_adj)−1] where log_β_adj expressed in log-adjusted ng·m⁻³/year for PAH;; boldface type indicates statistical significance with **p value <0.001.

Fig. 4. Temporal trends of residential indoor (a) pyrene and (b) Σ₈PAH_nonvolatile concentrations from 2001 to 2012, stratified by age group

Annual arithmetic mean concentrations of indoor PAH levels with 95% confidence interval are presented by age group.

Fig. 5. Temporal trends of (a) 2-naphthol and (b) 1-hydroxypyrene concentrations in urine from 2001 to 2012, stratified by age group

Annual arithmetic mean concentrations of specific gravity-adjusted metabolites with 95% confidence interval are presented by age group. Visual graphic representation was selected based on the significance of positive associations between year of monitoring and PAH metabolites shown in supplementary table 6.