Elsevier

Atmospheric Environment

Volume 86, April 2014, Pages 203-211
Atmospheric Environment

Temporal associations of ambient PM2.5 elemental concentrations with indoor and personal concentrations

https://doi.org/10.1016/j.atmosenv.2013.12.021Get rights and content

Highlights

  • Temporal associations of outdoor with indoor/personal concentrations were examined.

  • We investigated Cu, Zn, Fe, K, Ni, V, Si and S elemental concentrations of PM2.5.

  • High temporal correlations were found for most elements.

  • The highest correlations were found for S and V, the lowest for Cu.

Abstract

Time series studies increasingly evaluate health relevance of the elemental composition of particles smaller than 2.5 μm (PM2.5). Validation studies have documented that temporal variation of outdoor PM2.5 concentration is correlated with temporal variation of personal exposure, but very few papers have investigated the temporal correlation between outdoor concentration and personal exposure for the elemental composition of PM2.5. We evaluated the temporal association between outdoor concentration and personal exposure for the elements copper (Cu), zinc (Zn), iron (Fe), potassium (K), nickel (Ni), vanadium (V), silicon (Si) and sulfur (S) in three European cities.

In Helsinki (Finland), Utrecht (the Netherlands) and Barcelona (Spain) five participants from urban background, five from suburban/rural background and five from busy street sites were selected (15 participants per city). Six outdoor, indoor and personal 96-h average PM2.5 concentrations were measured simultaneously in three different seasons (winter, summer and spring/autumn). Concurrently, samples were collected at a central reference site, reflecting urban background air pollution levels. The temporal variation at the central site was highly correlated with personal exposure for all elements, except Cu. The highest correlations (Pearson's R) were found for S and V (R between 0.87 and 0.98). Lower correlations were found for the elements Cu, Fe and Si associated with non-tailpipe traffic emissions and road dust (Pearson's R between −0.34 and 0.79). For PM2.5 mass the R was lower (between 0.37 and 0.70). Exclusion of observations most affected by indoor sources increased the personal to central site correlations but did not fully explain differences between elements. The generally high correlation between temporal variation of the outdoor concentration and personal exposure supports the use of a central site for assessing exposure of PM components in time series studies for most elements. The different correlations found for the eight elements suggests that epidemiological associations are affected by differences in measurement error.

Introduction

Particulate matter with a diameter of less than 2.5 μm (PM2.5) has been associated with adverse health effects. However, less is known about which constituents of PM2.5 or which sources of particles are primarily responsible for these adverse health effects (Stanek et al., 2011, Kelly and Fussell, 2012, Rohr and Wyzga, 2012, Bell, 2012). The ambient concentrations of these components vary temporally due to changes in weather and emissions. For many epidemiologic air pollution time series studies, a central monitoring site is used to determine the exposure of study subjects. Previous studies have shown that the ambient concentrations of PM2.5 at a fixed site can be a good predictor for personal exposure, but the accuracy is dependent on the characteristics of participants, studies, and the environments in which they are conducted (Avery et al., 2010). Very few papers have investigated the short term temporal correlations between outdoor and personal elemental concentrations of PM2.5 (Janssen et al., 2005). A study in Amsterdam and Helsinki found that with the exception of sulfur and PM absorbance as a measure of Black Carbon, longitudinal correlations between personal and outdoor Cu, Zn, Fe, K, Ni, V, Si and S elemental concentrations were less than the correlations for PM2.5 which were 0.76 in Amsterdam and 0.74 in Helsinki (Janssen et al., 2005).

The aim of this paper is to assess the association between temporal variation in ambient concentrations of fine particle components at a central reference site and temporal variation in indoor and personal concentrations.

The study utilized repeated personal exposure measurements in Barcelona, Utrecht and Helsinki performed in the framework of the Validation of ESCAPE Exposure EstimateS using Personal exposure Assessment (VE3SPA) project (Montagne et al., 2013). VE3SPA was designed to evaluate how well land use regression models developed by the European Study of Cohorts for Air Pollution Effects (ESCAPE) project reflected spatial variation of outdoor, indoor and personal exposure (Eeftens et al., 2012b). The results for the spatial analyses have been published elsewhere for PM2.5, NO2 and soot (Montagne et al., 2013) and will be published elsewhere for the elemental composition.

Section snippets

Study design

PM2.5, soot (light absorbance of PM2.5 filters), NO2 and NOx were measured and the PM2.5 filters samples were chemically analyzed for elemental composition. Eight trace elements were a priori selected to represent different sources of air pollution, copper (Cu), zinc (Zn), iron (Fe), potassium (K), nickel (Ni), vanadium (V), silicon (Si) and sulfur (S). These eight elements were the elements selected in ESCAPE for land use regression modeling and epidemiological analysis (De Hoogh et al., 2013

Quality control

For most elements, more than 75% of the samples exceeded the detection limit (Table 1). For zinc (Zn) this percentage was slightly lower (68%), but was 100% if one extreme blank was excluded. This high blank measurement was excluded in all analyses. The coefficients of variance (CV) for the duplicate measurements, including the personal duplicate measurements, are shown in Table 2. CV values were fairly high, often exceeding 20%.

Descriptive results

The median, first and third quartile concentrations for the

Correlations with elemental exposure

Central site concentrations correlated well with home outdoor concentrations. Correlations were higher for S and V than for Cu, Fe and Si. The latter elements reflect the tail of coarse particles, which have more local sources compared to fine particles and therefore show different temporal patterns at different sites (close/far away from source) (Puustinen et al., 2007).

A statistically significant temporal relationship of the concentrations at a central site with personal concentrations was

Acknowledgments

The authors thank the volunteers for their participation and dedication in the project. The project was funded by Concawe (conservation of clean air and water in Europe), contract number 200907200, date 20-07-09.

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