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. A mobile laboratory equipped with state-of-the-art gaseous and particulateinstrumentation was deployed across the Greater Toronto Area (GTA) during twoseasons. A high-resolution time-of-flight chemical ionization mass spectrometer (HR-TOF-CIMS)measured isocyanic acid (HNCO) and hydrogen cyanide (HCN), and ahigh-sensitivity laser-induced incandescence (HS-LII) instrument measuredblack carbon (BC). Results indicate that on-road vehicles are a clear sourceof HNCO and HCN and that their impact is more pronounced in the winter, wheninfluences from biomass burning (BB) and secondary photochemistry are weakest.Plume-based and time-based algorithms were developed to calculatefleet-average vehicle emission factors (EFs); the algorithms were found toyield comparable results, depending on the pollutant identity. With respectto literature EFs for benzene, toluene, C2 benzene (sum of m-, p-, and o-xylenes andethylbenzene), nitrogen oxides, particle number concentration (PN), and blackcarbon, the calculated EFs were characteristic of a relatively clean vehiclefleet dominated by light-duty vehicles (LDV). Our fleet-average EF for BC (median:25 mg kg fuel - 1 ; interquartile range, IQR:10–76 mg kg fuel - 1 ) suggests that overall vehicularemissions of BC have decreased over time. However, the distribution of EFsindicates that a small proportion of high-emitters continue to contributedisproportionately to total BC emissions. We report the first fleet-averageEF for HNCO (median: 2.3 mg kg fuel - 1 , IQR:1.4–4.2 mg kg fuel - 1 ) and HCN (median:0.52 mg kg fuel - 1 , IQR:0.32–0.88 mg kg fuel - 1 ). The distribution of the estimatedEFs provides insight into the real-world variability of HNCO and HCNemissions and constrains the wide range of literature EFs obtained fromprior dynamometer studies. The impact of vehicle emissions on urban HNCOlevels can be expected to be further enhanced if secondary HNCO formationfrom vehicle exhaust is considered.

atmospheric chemistry and physics

Elucidating real-world vehicle emission factors from mobile measurements over a large metropolitan region: a focus on isocyanic acid, hydrogen cyanide, and black carbon