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Environmental Modeling

Using Mobile Monitoring to Develop Hourly Empirical Models of Particulate Air Pollution in a Rural Appalachian Community Steve Hankey, Peter Sforza, and Matt Pierson Environ. Sci. Technol., Just Accepted Manuscript • Publication Date (Web): 15 Mar 2019 Downloaded from http://pubs.acs.org on March 15, 2019

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Environmental Science & Technology

Using Mobile Monitoring to Develop Hourly Empirical Models of Particulate Air Pollution in a Rural Appalachian Community

Steve Hankey,1* Peter Sforza,2 Matt Pierson2 1School

of Public and International Affairs, Virginia Tech, 140 Otey Street, Blacksburg, VA

24061 2Center

for Geospatial Information Technology, Virginia Tech, 620 Drillfield Drive, Blacksburg, VA 24061 *Corresponding Author: email: [email protected]; phone: 540.231.7508. Word count: 4,874 + 300×4 small tables/figures + 600×2 large tables/figures = 7,274 Submitted: March 13, 2019

KEYWORDS traffic-related air pollution; ultrafine particles; particle number concentration; land use regression

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ABSTRACT

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Most empirical air quality models (e.g., land use regression) focus on urban areas.

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Mobile monitoring for model development offers the opportunity to explore smaller, rural

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communities – an understudied population. We use mobile monitoring to systematically sample

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all daylight hours (7am-7pm) to develop empirical models capable of estimating hourly

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concentrations in Blacksburg, VA – a small town in rural Appalachia (population: 182,635). We

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collected ~120 hours of mobile monitoring data for Particle Number (PN) and Black Carbon

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(BC). We developed (1) daytime (12-hour average) models that approximate long-term

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concentrations and (2) spatiotemporal models for estimating hourly concentrations. Model

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performance for the daytime models is consistent with previous fixed-site and short-term

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sampling studies; adjusted R2 (10-fold CV R2) was 0.80 (0.69) for the PN model and 0.67 (0.58)

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for the BC model. The spatiotemporal models had comparable performance (10-fold CV R2 for

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the PN [BC] models: 0.42 [0.25]) to previous mobile monitoring studies that isolate specific time

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periods. Temporal and spatial model coefficients had similar magnitudes in the spatiotemporal

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models suggesting both factors are important for exposure. We observed similar spatial patterns

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in Blacksburg (e.g., roadway gradients) as in other studies in urban areas suggesting similar

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exposure disparities exist in small, rural communities.

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TOC Art

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INTRODUCTION Empirical models of air quality have traditionally employed fixed-site monitoring to

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estimate annual-average concentrations for model building 1-2. Air quality researchers have

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primarily focused on improving the spatial precision of empirical models of air quality (e.g., land

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use regression [LUR]) to estimate long-term average concentrations 3-5 for use in health effects

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studies 6-7. Recent work has added temporal resolution by modeling monthly 8-9 or daily 10

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average concentrations. Emerging work has explored use of mobile monitoring to develop

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models with hourly resolution 11. Most of these empirical models focus on urban areas. The US

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Census estimates that ~29 million people (or ~9% of the US population) live in 199 Metropolitan

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Statistical Areas (MSA) of < 250,000 people (~50% of the total MSAs) 12. An understudied topic

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is development of empirical models in these relatively smaller communities where little air

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quality monitoring data is available. More work is needed to assess whether trends from previous

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empirical modeling studies in urban areas are consistent with or differ for smaller communities.

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An increasing number of studies use mobile monitoring to characterize specific traffic

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corridors 13-15, develop and assess empirical models 16-21, and apply those models for

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epidemiological studies 22. Use of mobile monitoring may be particularly useful for pollutants

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with high spatial and temporal variability 23. Some studies have compared empirical models

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developed using mobile monitoring vs. fixed-site monitoring 24-27 or assessed merging mobile

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monitoring with fixed-site monitoring to develop spatiotemporal models 28; however, results of

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these comparisons vary by study and the amount of mobile and fixed-site data collected. Since

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mobile monitoring is typically conducted across many days (and various times of day), previous

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studies have used a variety of methods to adjust mobile monitoring data for background

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concentrations 11, 16, 27, 29. An understudied topic is how the choice of background adjustment

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method impacts model performance and the spatial patterns of modeled concentration estimates.

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Accurately assessing human exposure to air pollution depends on correctly estimating the

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spatiotemporal patterns of pollutant concentrations to match people’s time-activity patterns 30-33.

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In this study, we present results of spatiotemporal empirical models of particulate air pollution

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for the rural Appalachian community of Blacksburg, VA based on mobile monitoring of Particle

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Number (PN) and Black Carbon (BC) concentrations – pollutants that have high spatial

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variability in urban environments 34-38 and are associated with health disparities at small spatial

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scales 39-42. We develop a number of empirical models to test how inclusion of temporal

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variables (e.g., meteorology, time of day) and type of background concentration correction

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impact model performance. We focus on comparing how model-derived short-term (hourly)

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concentration estimates compare to long-term (daily) estimates to assess how choice of spatial or

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spatiotemporal modeling approach impacts exposure assessment.

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MATERIALS AND METHODS

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Our work employs mobile monitoring during the daylight hours (7am-7pm) of the

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summer and fall of year-2016 for the purpose of developing empirical models of particulate air

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pollution with hourly time resolution. Our study area is a small rural town in the Blue Ridge

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Mountains (Blacksburg, VA; MSA population: 182,635).

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Mobile monitoring data

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Mobile monitoring platform

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We developed a custom mobile monitoring platform to collect spatially and temporally

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resolved measurements of PN and BC (Figure 1). The platform consists of (1) a CPC 3007 (TSI,

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Inc.) to measure PN, (2) a micro-aethalometer (AE51; AethLabs) to measure BC, (3) a

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Raspberry Pi and GPS antenna, and (4) an external battery. The platform logs and geo-locates

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measurements every second. The Raspberry Pi includes a WiFi antenna to transfer all monitoring

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data to a server when a WiFi signal is present. All post-processing Python scripts are run on a

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server prior to making the data available for download on a website (details on the procedures

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included in the post-processing script is below) which allowed for viewing time series and

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mapped data for each monitoring run. (The Python script is available upon request from the

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corresponding author.) The platform is mounted to a bicycle rack on an electric assist bicycle for

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mobile monitoring; an elevated air intake was used to sample at approximately the breathing

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height of a cyclist or pedestrian. The monitoring platform is in Figure 1; further details are in

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Figures S1-S3.

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[Insert Figure 1 about here] Mobile monitoring campaign We selected two mobile monitoring routes with the goal of spanning a variety of

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environments that may impact PN and BC concentrations (Figure S4). Each route was ~20

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kilometers in length and could be completed in ~45-60 minutes. We chose the sampling routes to

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sample various road types (major and minor roads, off-street trails), land uses (residential,

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commercial, natural environments), and emission sources (heavy- and light-duty vehicle

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volumes).

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Core goals of our work are (1) to compare short- and long-term concentration estimates

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of empirical models developed using mobile monitoring data, (2) test how inclusion of various

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meteorological variables and background concentration adjustments impact model performance,

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and (3) explore spatial trends in a small, rural Appalachian town. We stratified mobile

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monitoring by hour of day. Specifically, we completed each sampling route a minimum of 5

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times per hour of day from 7am-7pm (Figure S5) resulting in ~10 hours (2 routes × 5 sampling

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runs × 1 hour per sampling run) of mobile monitoring data per hour of the day for model

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building. In total, we collected ~120 hours (12 hours of day × 10 hours of monitoring data per

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hour) of data during the mobile monitoring campaign.

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Central site measurements and monitor calibration

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We monitored PN (CPC 3783; TSI, Inc.) and BC (AE51; Aethlabs) at a central site for

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the entire monitoring campaign (7/20/2016 – 10/23/2016). We added a particle size selector

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(TSI, Inc.) to the CPC 3783 (cutoff size: 7 nm) to match the 10 nm cutoff size of the CPC 3007.

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The central site was located where all mobile monitoring routes began and finished (Figure S6);

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measurements were logged in 1-minute intervals. We used the central site measurements to

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correct all mobile measurements for variation in background concentrations (see below). We co-

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located all monitoring equipment at a near-road location for 22 hours (among 4 days) before and

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14 hours (among 3 days) after the mobile monitoring campaign. We used data from the co-

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located monitoring to correct all measurements to a reference CPC and micro-aethalometer.

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Figures S7-S12 and Table S1 give further details on the results of the co-location analysis.

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Processing measurement data for spatial modeling

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Below we briefly describe data processing for the mobile monitoring data (further detail

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is in the SI).

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Measurement corrections and data processing

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Monitor co-location corrections. Based on the co-location measurements, we developed

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instrument-specific correction factors to adjust all mobile monitoring data to a reference CPC

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and micro-aethalometer. The corrections resulted in an average correction factor of 1.09 for the

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CPCs and 0.98 for the micro-aethalometers. We applied a time delay correction as observed in

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our previous mobile monitoring study with a similar monitoring platform 16, 43 (Table S2).

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Micro-aethalometer corrections. We corrected all BC measurements for two known

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artifacts of sampling: (1) particle loading on the micro-aethalometer filter and (2) spurious data

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associated with mechanical shock. We followed Kirchstetter and Novakov 44 to adjust for

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particle loading and Apte et al. 45 to identify and remove spurious data from mechanical shock.

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This procedure resulted in removal of 10% of the mobile monitoring data. We collected BC

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measurements on a 1 second basis but temporally smoothed the data on a 60s basis due to

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inherent noise associated with the micro-aethalometer.

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CPC corrections. We corrected PN measurements from the CPC 3007 for undercounting

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at high concentrations (>100,000 pt/cc). We used the correction equation developed by

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Westerdahl et al. 46. Our near-road, co-located measurements demonstrated a similar relationship

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as reported by Westerdahl et al. 46 (Figure S12); we chose to apply the previously published

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correction equation since those measurements were collected in a variety of locations rather than

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a single near-road location.

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Background adjustments. To test the impact of day-to-day variability in background

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concentrations we developed models using three scenarios (1) mobile monitoring data

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unadjusted for background concentrations, (2) an additive background adjustment similar to

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Hankey and Marshall 16, and (3) a multiplicative background adjustment as described in Apte et

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al. 29.

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For the additive adjustment, we first applied a 60-minute temporal smoothing to the

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central site data. Then, we subtracted the background concentration estimate from each

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corresponding mobile monitoring observation (leaving only the local, on-road concentration

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component of each measurement). Upon completion of the entire monitoring campaign we

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calculated an average hourly background concentration and added that value to each on-road

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concentration estimate for the corresponding hour for use in model building. This background

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adjustment aims to adjust concentration estimates to reflect the average temporal background

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concentration trends during our study period which may better reflect typical patterns rather than

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trends specific to days where mobile monitoring data was collected.

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For the multiplicative adjustment, we developed correction factors with more temporal

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resolution than the additive adjustment. First, we calculated the median concentration for each

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mobile monitoring day for all daylight hours (7am-7pm) at the central site. We also calculated

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the median central site concentration for each hour of day. The correction factor for each mobile

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monitoring observation was calculated as the ratio of the daily concentration to the hourly

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concentration. This correction has superior temporal resolution to the additive background

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adjustment; however, it is likely best suited for estimating daily concentrations since the

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correction adjusts all mobile monitoring observations to the daily median value. Distributions of

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unadjusted and background adjusted concentrations are shown in Figures S13-S15.

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Spatial aggregation

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We spatially aggregated the mobile monitoring data as the core input to the empirical

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models described below. We first snapped all mobile measurements to aggregation points

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created at 100 meter intervals along the monitoring routes. Then, we tabulated median

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concentrations at each aggregation location to minimize the impact of outlier values and to

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follow on our previous work 16. We performed this aggregation for all mobile monitoring data

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during all daylight hours (7am-7pm; ~931 observations per aggregation location) and for each

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individual hour of day (~77 observations per aggregation location). This procedure resulted in

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423 locations with concentration estimates for model development (Table S3; Figure S16).

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Database of covariates for spatial modeling

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We tabulated a variety of candidate covariates that measure land use, the transportation

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network, and the natural environment (Table 1). All variables were tabulated at 15 buffer sizes

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(25 – 3,000 meters) and were included in the model selection process. All underlying data was

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from publicly available sources with the exception of traffic volumes. To estimate traffic

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volumes across the network we used existing traffic counts to develop statistical models to

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estimate annual-average daily traffic for the entire network; we developed separate models for

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heavy- and light-duty vehicles (Tables S4-S5). We also included hour of day (as a dummy

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variable) and 5 meteorological parameters (temperature, relative humidity, planetary boundary

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layer, precipitation, wind speed) in the spatiotemporal models.

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[Insert Table 1 about here]

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Modeling approach

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We developed three sets of models to compare short- and long-term concentration

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estimates from empirical models developed using mobile monitoring: (1) daytime models which

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aggregate all mobile monitoring data to approximate traditional, fixed-site empirical models

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(e.g., LUR), (2) single-hour models which develop a single model for each hour of the day, and

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(3) spatiotemporal models that include time of day and meteorological parameters as candidate

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variables for selection in a single model to estimate hourly concentrations.

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We employed the stepwise regression approach originally developed by Su et al. 47 and

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applied to mobile monitoring data by Hankey and Marshall 16 using MATLAB R2017b. Briefly,

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model selection proceeds by adding variables most correlated with the dependent variables (PN

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and BC concentrations), and subsequently most correlated with model residuals. The model

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building process is terminated when a variable is either not significant in the model (p