Incorporation of lumped IVOC emissions into the ORACLE model (V1.1): A multi-product framework for assessing global SOA formation from internal combustion engines
Abstract. Secondary organic aerosol (SOA) is a major component of particulate matter but is often underpredicted in chemistry climate models. Recent advances in measuring and resolving the chemically complex structure of intermediate volatile organic compounds (IVOC) have shown that IVOCs, despite their high SOA yields, have long been underrepresented in models. These compounds are key precursors of SOA from emissions in the road transport sector and significantly influence SOA formation. Understanding vehicle emissions, their chemistry, and their SOA-forming potential is essential for accurately estimating their contributions to atmospheric SOA and global organic aerosol loads. To improve this understanding, we have updated the organic module ORACLE in the global chemistry climate model EMAC. The existing IVOC representation was based on scaled organic carbon (OC) emissions and a highly parameterized volatility basis set (VBS) which underestimated global IVOC emissions and oversimplified their chemistry. Here, we replaced this approach with a lumped species framework, in which experimental data for gasoline and diesel emissions were grouped into seven lumped species based on their chemical properties and hydroxylation potentials. These species were linked to adjusted emission inventories for regional diesel and gasoline consumption. A 10-year simulation with the updated ORACLE-IVOC model resulted in significant changes. The global atmospheric burden of road transport IVOC-derived SOA (SOA-iv) increased by 1 order of magnitude, from 0.014 Tg to 0.13 Tg. The composition of road transport organic aerosol (OA) shifted, with SOA-iv contributing 2.5 to 13 times more than the primary organic aerosol (POA) and SOA derived from semi-volatile organic compounds combined. In the results using the previous model, this ratio was between 0.4 and 1.1. The geographical distribution of OA also changed. Regions rich in gasoline relative to diesel emissions experienced higher concentration increases, and remote areas experienced elevated concentrations due to more efficient long-range transport of the new lumped IVOC species. Overall, these changes led to a significant increase in the contribution of road transport to total anthropogenic SOA-iv from an average value of 3 % to 35 %.
In this study, the authors have updated the organic module ORACLE in the global model EMAC by adding the SOA aging process from seven lumped IVOC precursor groups. A new road transport IVOC emission inventory with chemical speciation was also established and input into the updated model. However, given that there is already sufficient research basis on IVOC emission factors by vehicle type and emission standard, the newly established road transport IVOC emission inventory appears to be rather coarse. Moreover, the authors did not demonstrate the superiority of the new model compared to previous models, such as its better alignment with the observations. Overall, this study needs establishment of a more detailed emission inventory, and careful consideration of scenario design to more clearly discuss the significance of the new mechanism and the new inventory, to draw more scientifically robust and reliable conclusions.