A temporally and spatially resolved validation of emission inventories by measurements of ambient volatile organic compounds in Beijing, China

Abstract. Understanding the sources of volatile organic compounds (VOCs) is essential for ground-level ozone and secondary organic aerosol (SOA) abatement measures. We made VOC measurements at 27 sites and online observations at an urban site in Beijing from July 2009 to January 2012. Based on these measurement data, we determined the spatial and temporal distribution of VOCs, estimated their annual emission strengths based on their emission ratios relative to carbon monoxide (CO), and quantified the relative contributions of various sources using the chemical mass balance (CMB) model. These results from ambient measurements were compared with existing emission inventories to evaluate the spatial distribution, species-specific emissions, and source structure of VOCs in Beijing. The measured VOC distributions revealed a hotspot in the southern suburban area of Beijing, whereas current emission inventories suggested that VOC emissions were concentrated in downtown areas. Compared with results derived from ambient measurements, the annual inventoried emissions of oxygenated VOC (OVOC) species and C2–C4 alkanes may be underestimated, while the emissions of styrene and 1,3-butadiene may be overestimated by current inventories. Source apportionment using the CMB model identified vehicular exhaust as the most important VOC source, with the relative contribution of 49%, in good agreement with the 40–51% estimated by emission inventories. The relative contribution of paint and solvent utilization obtained from the CMB model was 14%, significantly lower than the value of 32% reported by one existing inventory. Meanwhile, the relative contribution of liquefied petroleum gas (LPG) usage calculated using the CMB model was 6%, whereas LPG usage contribution was not reported by current emission inventories. These results suggested that VOC emission strengths in southern suburban area of Beijing, annual emissions of C2–C4 alkanes, OVOCs and some alkenes, and the contributions of solvent and paint utilization and LPG usage in current inventories all require significant revisions.