Deriving emission fluxes of volatile organic compounds from tower observation in the Pearl River Delta, China

Accurate estimation of speciated emissions of volatile organic compounds (VOCs) is challenging due to the complexity of both species and sources. Evaluation of the bottom-up emission inventory (EI) by atmospheric observation is needed to better understand the VOC emissions and then to control air pollutions caused by VOCs. This study conducts vertical measurements of VOCs between November 3 and 11, 2018 at the Canton Tower in the urban core of Pearl River Delta (PRD), China. A mixed layer gradient (MLG) technique is applied to the tower observation data to derive emission fluxes for individual VOC. The results show that the measured VOCs concentrations at ground level were always higher than those at the heights of 118 m and 488 m. Obvious vertical gradients of concentrations were found for VOC species, such as benzene, toluene and isoprene. The emission flux was estimated to be largest for propane (3.29 mg m^-2 h^-1), followed by toluene (2.55 mg m^-2 h^-1), isoprene (2.24 mg m^-2 h^-1), n-butane (2.10 mg m^-2 h^-1) and iso-pentane (1.73 mg m^-2 h^-1). The total VOC emission fluxes were around 3 times larger than those in the EI, suggesting 1.5-2 times underestimations of ozone formation potential (OFP) and secondary organic aerosol potential (SOAP) by current EI. Substantial underestimations (3-20 times) were found for C₂-C₅ alkanes by current EI. Due to unmeasured input parameters, limited sample size and short sampling period, there are still large uncertainties (40%-117%) in the estimated emission fluxes for individual species. Whereas, this study shows that the tower observation and emission estimation using MLG method could provide useful information for better understanding vertical distributions and emission fluxes of VOCs, and pioneer in assessing the existing emission inventories at species-level and hour-level.