Abstract

Despite advances in monitoring and modelling of intra-urban variation in multiple pollutants, few studies have attempted to separate spatial patterns by time of day, or incorporated organic tracers into spatial monitoring studies. Due to varying emissions sources from diesel and gasoline vehicular traffic, as well as within-day temporal variation in source mix and intensity (e.g., rush-hours vs. full-day measures), accurately assessing diesel-related air pollution within an urban core can be challenging. We allocated 24 sampling sites across downtown Pittsburgh, Pennsylvania (2.8 km2) to capture fine-scale variation in diesel-related pollutants, and to compare these patterns by sampling interval (i.e., “rush-hours” vs. “work-week” concentrations), and by season. Using geographic information system (GIS)-based methods, we allocated sampling sites to capture spatial variation in key traffic-related pollution sources (i.e., truck, bus, overall traffic densities). Programmable monitors were used to collect integrated work-week and rush-hour samples of fine particulate matter (PM2.5), black carbon (BC), trace elements, and diesel-related organics (polycyclic aromatic hydrocarbons (PAHs), hopanes, steranes), in summer and winter 2014. Land use regression (LUR) models were created for PM2.5, BC, total elemental carbon (EC), total organic carbon (OC), elemental (Al, Ca, Fe), and organic constituents (total PAHs, total hopanes), and compared by sampling interval and season. We hypothesized higher pollution concentrations and greater spatial contrast in rush-hour, compared to full work-week samples, with variation by season and pollutant. Rush-hour sampling produced slightly higher total PM2.5 and BC concentrations in both seasons, compared to work-week sampling, but no evident difference in spatial patterns. We also found substantial spatial variability in most trace elements and organic compounds, with comparable spatial patterns using both sampling paradigms. Overall, we found higher concentrations of traffic-related trace elements and organic compounds in rush-hour samples, and higher concentrations of coal-related elements (e.g., As, Se) in work-week samples. Mean bus density was the strongest LUR predictor in most models, in both seasons, under each sampling paradigm. Within each season and constituent, the bus-related terms explained similar proportions of variance in the rush-hour and work-week samples. Rush-hour and work-week LUR models explained similar proportions of spatial variation in pollutants, suggesting that the majority of emissions may be produced during rush-hour traffic across downtown. Results suggest that rush-hour emissions may predominantly shape overall spatial variance in diesel-related pollutants.

Highlights

  • Despite improvements in monitoring and modelling of intra-urban variation in multiple air pollutants, few studies have attempted to separate spatial patterns by time of day, or to incorporate organic tracers for key emissions sources [1]

  • Spatial patterning in PMdifferences was similar, with generally higherorconcentrations

  • While rush-hour sampling produced slightly higher PM2.5 concentrations, there were no evident differences in spatial patterns, compared to work-week sampling, and rush-hour and work-week land use regression (LUR) models explained similar proportions of variability in concentrations in each season

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Summary

Introduction

Despite improvements in monitoring and modelling of intra-urban variation in multiple air pollutants, few studies have attempted to separate spatial patterns by time of day, or to incorporate organic tracers for key emissions sources [1]. Many studies have captured fine-scale spatial variation in urban air pollution, and successfully applied land use regression (LUR) and related spatial modelling methods to estimate exposures and to support identification of key sources [6,7,8]. There have been substantial improvements in methods for multi-pollutant saturation monitoring [10], relatively few spatial studies have incorporated source-specific organic particle components [11,12,13], in part due to the greater volatility and instability of these compounds.

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