Abstract. On-road vehicle emissions are a major contributor to elevated air pollution levels in populous metropolitan areas. We developed a link-level emissions inventory of vehicular pollutants, called EMBEV-Link (Link-level Emission factor Model for the BEijing Vehicle fleet), based on multiple datasets extracted from the extensive road traffic monitoring network that covers the entire municipality of Beijing, China (16 400 km2). We employed the EMBEV-Link model under various traffic scenarios to capture the significant variability in vehicle emissions, temporally and spatially, due to the real-world traffic dynamics and the traffic restrictions implemented by the local government. The results revealed high carbon monoxide (CO) and total hydrocarbon (THC) emissions in the urban area (i.e., within the Fifth Ring Road) and during rush hours, both associated with the passenger vehicle traffic. By contrast, considerable fractions of nitrogen oxides (NOx), fine particulate matter (PM2.5) and black carbon (BC) emissions were present beyond the urban area, as heavy-duty trucks (HDTs) were not allowed to drive through the urban area during daytime. The EMBEV-Link model indicates that nonlocal HDTs could account for 29 % and 38 % of estimated total on-road emissions of NOx and PM2.5, which were ignored in previous conventional emission inventories. We further combined the EMBEV-Link emission inventory and a computationally efficient dispersion model, RapidAir®, to simulate vehicular NOx concentrations at fine resolutions (10 m × 10 m in the entire municipality and 1 m × 1 m in the hotspots). The simulated results indicated a close agreement with ground observations and captured sharp concentration gradients from line sources to ambient areas. During the nighttime when the HDT traffic restrictions are lifted, HDTs could be responsible for approximately 10 µg m−3 of NOx in the urban area. The uncertainties of conventional top-down allocation methods, which were widely used to enhance the spatial resolution of vehicle emissions, are also discussed by comparison with the EMBEV-Link emission inventory.

Abstract. Although secondary particulate matter is reported to be the main contributor of PM2.5 during haze in Chinese megacities, primary particle emissions also affect particle concentrations. In order to improve estimates of the contribution of primary sources to the particle number and mass concentrations, we performed source apportionment analyses using both chemical fingerprints and particle size distributions measured at the same site in urban Beijing from April to July 2018. Both methods resolved factors related to primary emissions, including vehicular emissions and cooking emissions, which together make up 76 % and 24 % of total particle number and organic aerosol (OA) mass, respectively. Similar source types, including particles related to vehicular emissions (1.6±1.1 µg m−3; 2.4±1.8×103 cm−3 and 5.5±2.8×103 cm−3 for two traffic-related components), cooking emissions (2.6±1.9 µg m−3 and 5.5±3.3×103 cm−3) and secondary aerosols (51±41 µg m−3 and 4.2±3.0×103 cm−3), were resolved by both methods. Converted mass concentrations from particle size distributions components were comparable with those from chemical fingerprints. Size distribution source apportionment separated vehicular emissions into a component with a mode diameter of 20 nm (“traffic-ultrafine”) and a component with a mode diameter of 100 nm (“traffic-fine”). Consistent with similar day- and nighttime diesel vehicle PM2.5 emissions estimated for the Beijing area, traffic-fine particles, hydrocarbon-like OA (HOA, traffic-related factor resulting from source apportionment using chemical fingerprints) and black carbon (BC) showed similar diurnal patterns, with higher concentrations during the night and morning than during the afternoon when the boundary layer is higher. Traffic-ultrafine particles showed the highest concentrations during the rush-hour period, suggesting a prominent role of local gasoline vehicle emissions. In the absence of new particle formation, our results show that vehicular-related emissions (14 % and 30 % for ultrafine and fine particles, respectively) and cooking-activity-related emissions (32 %) dominate the particle number concentration, while secondary particulate matter (over 80 %) governs PM2.5 mass during the non-heating season in Beijing.

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