High-resolution spatial and spatiotemporal modelling of air pollution using fixed site and mobile monitoring in a Canadian city.

The development of high-resolution spatial and spatiotemporal models of air pollutants is essential for exposure science and epidemiological applications. While fixed-site sampling has conventionally provided input data for statistical predictive models, the evolving mobile monitoring method offers improved spatial resolution, ideal for measuring pollutants with high spatial variability such as ultrafine particles (UFP). The Quebec Air Pollution Exposure and Epidemiology (QAPEE) study measured and modelled the spatial and spatiotemporal distributions of understudied pollutants, such as UFPs, black carbon (BC), and brown carbon (BrC), along with fine particulate matter (PM2.5), nitrogen dioxide (NO2), and ozone (O3) in Quebec City, Canada. We conducted a combined fixed-site (NO2 and O3) and mobile monitoring (PM2.5, BC, BrC, and UFPs) campaign over 10-months. Mobile monitoring routes were monitored on a weekly basis between 8am-10am and designed using location/allocation modelling. Seasonal fixed-site sampling campaigns captured continuous 24-h measurements over two-week periods. Generalized Additive Models (GAMs), which combined data on pollution concentrations with spatial, temporal, and spatiotemporal predictor variables were used to model and predict concentration surfaces. Annual models for PM2.5, NO2, O3 as well as seven of the smallest size fractions in the UFP range, had high out of sample predictive accuracy (range r2: 0.54-0.86). Varying spatial patterns were observed across UFP size ranges measured as Particle Number Counts (PNC). The monthly spatiotemporal models for PM2.5 (r2 = 0.49), BC (r2 = 0.27), BrC (r2 = 0.29), and PNC (r2 = 0.49) had moderate or moderate-low out of sample predictive accuracy. We conducted a sensitivity analysis and found that the minimum number of 'n visits' (mobile monitoring sessions) required to model annually representative air pollution concentrations was between 24 and 32 visits dependent on the pollutant. This study provides a single source of exposure models for a comprehensive set of air pollutants in Quebec City, Canada. These exposure models will feed into epidemiological research on the health impacts of ambient UFPs and other pollutants.

Evaluating the effectiveness of low-sulphur marine fuel regulations at improving urban ambient PM2.5 air quality: Source apportionment of PM2.5 at Canadian Atlantic and Pacific coast cities with implementation of the North American Emissions Control Area.

Ambient fine size fraction particulate matter (PM2.5) sources were resolved by positive matrix factorization at two Canadian cities on the Atlantic and Pacific coast over the 2010-2016 period, corresponding to implementation of the North American Emissions Control Area (NA ECA) low-sulphur marine fuel regulations. Source types contributing to local PM2.5 concentrations were: ECA regulation-related (residual oil, anthropogenic sulphate), urban transportation and residential (gasoline, diesel, secondary nitrate, biomass burning, road dust/soil), industry (refinery, Pb-enriched), and largely natural (biogenic sulphate, sea salt). Anthropogenic sources accounted for approximately 80 % of PM2.5 mass over 2010-2016. Anthropogenic and biogenic sources of PM2.5-sulphate were separated and apportioned. Anthropogenic PM2.5-sulphate was approximately 2-3 times higher than biogenic PM2.5-sulphate prior to implementation of the NA ECA low-S marine fuel regulations, decreasing to 1-2 times higher after regulation implementation. Non-marine anthropogenic sources (gasoline, road dust, local industry factors) were shown to together contribute 38 % - 45 % of urban PM2.5. At both coastal cities, the residual oil and anthropogenic sulphate factors clearly reflected the effects of the low-S fuel regulations at reducing primary and secondary sulphur-related PM2.5 emissions. Comparing a pre-regulation and post-regulation period, residual oil combustion PM2.5 decreased by 0.24-0.25 µg/m3 (94%-95 % decrease) in both cities and anthropogenic sulphate PM2.5 decreased by 0.78 µg/m3 in Halifax (47 % decrease) and 0.71 µg/m3 in Burnaby (58 % decrease). Regulation-related PM2.5 across these factors decreased by approximately 1 µg/m3 after regulation implementation, providing a quantified lower estimate of the beneficial influence of the regulations on urban ambient PM2.5 concentrations. Further reductions in coastal city ambient PM2.5 may best consider air quality strategies that include multiple sources, including marine shipping and non-marine anthropogenic source types given this analysis found that marine vessel emissions remain an important source of urban ambient PM2.5.

Predicting intraurban airborne PM1.0-trace elements in a port city: Land use regression by ordinary least squares and a machine learning algorithm.

Airborne particulate matter (PM) has been associated with cardiovascular and respiratory morbidity and mortality, and there is some evidence that spatially varying metals found in PM may contribute to adverse health effects. We developed spatially refined models for PM trace elements using ordinary least squares land use regression (OLS-LUR) and machine leaning random forest land-use regression (RF-LUR). Two-week integrated measurements of PM1.0 (median aerodiameter < 1.0 µm) were collected at 50 sampling sites during fall (2010), winter (2011), and summer (2011) in the Halifax Regional Municipality, Nova Scotia, Canada. PM1.0 filters were analyzed for metals and trace elements using inductively coupled plasma-mass spectrometry. OLS- and RF-LUR models were developed for approximately 30 PM1.0 trace elements in each season. Model predictors included industrial, commercial, and institutional/ government/ military land use, roadways, shipping, other transportation sources, and wind rose information. RF generated more accurate models than OLS for most trace elements based on 5-fold cross validation. On average, summer models had the highest cross validation R2 (OLS-LUR = 0.40, RF-LUR = 0.46), while fall had the lowest (OLS-LUR = 0.27, RF-LUR = 0.31). Many OLS-LUR models displayed overprediction in the final exposure surface. In contrast, RF-LUR models did not exhibit overpredictions. Taking overpredictions and cross validation performances into account, OLS-LUR performed better than RF-LUR in roughly 20% of the seasonal trace element models. RF-LUR models provided more interpretable predictors in most cases. Seasonal predictors varied, likely due to differences in seasonal distribution of trace elements related to source activity, and meteorology.