摘要
Currently, modeling studies tend to significantly underestimate observed space-based glyoxal （CHOCHO） vertical column densities （VCDs）, implying the existence of missing sources of giyoxal. Several recent studies suggest that the emissions of aromatic compounds and molar yields of glyoxal in the chemical mechanisms may both be underestimated, which can affect the simulated glyoxal concentrations. In this study, the influences of these two factors on glyoxal amounts over China were investigated using the RAMS-CMAQ modeling system for January and July 2014. Four sensitivity simulations were performed, and the results were compared to satellite observations. These results demonstrated significant impacts on glyoxal concentrations from these two factors. In case 1, where the emissions of aromatic compounds were increased three-fold, improvements to glyoxal VCDs were seen in high anthropogenic emissions regions. In case 2, where molar yields of glyoxal from isoprene were increased five-fold, the resulted concentrations in July were B-B-fold higher, achieving closer agreement between the modeled and measured glyoxal VCDs. The combined changes from both cases 1 and 2 were applied in case B, and the model succeeded in further reducing the underestimations of glyoxal VCDs. However, the results over most of the regions with pronounced anthropogenic emissions were still underestimated. So the molar yields of giyoxal from anthropogenic precursors were considered in case 4. With these additional mole yield changes （a two-fold increase）, the improved concentrations agreed better with the measurements in regions of the lower reaches of the Yangtze River and Yellow River in January but not in July.
Currently, modeling studies tend to significantly underestimate observed space-based glyoxal （CHOCHO） vertical column densities （VCDs）, implying the existence of missing sources of giyoxal. Several recent studies suggest that the emissions of aromatic compounds and molar yields of glyoxal in the chemical mechanisms may both be underestimated, which can affect the simulated glyoxal concentrations. In this study, the influences of these two factors on glyoxal amounts over China were investigated using the RAMS-CMAQ modeling system for January and July 2014. Four sensitivity simulations were performed, and the results were compared to satellite observations. These results demonstrated significant impacts on glyoxal concentrations from these two factors. In case 1, where the emissions of aromatic compounds were increased three-fold, improvements to glyoxal VCDs were seen in high anthropogenic emissions regions. In case 2, where molar yields of glyoxal from isoprene were increased five-fold, the resulted concentrations in July were B-B-fold higher, achieving closer agreement between the modeled and measured glyoxal VCDs. The combined changes from both cases 1 and 2 were applied in case B, and the model succeeded in further reducing the underestimations of glyoxal VCDs. However, the results over most of the regions with pronounced anthropogenic emissions were still underestimated. So the molar yields of giyoxal from anthropogenic precursors were considered in case 4. With these additional mole yield changes （a two-fold increase）, the improved concentrations agreed better with the measurements in regions of the lower reaches of the Yangtze River and Yellow River in January but not in July.
基金
supported by the National Natural Science Foundation of China (No. 91544221)
the National Key R&D Programs of China (Nos. 2017YFC0209803, 2017YFC0210000)
the CAS Strategic Priority Research Program Grant (No. XDB05020000)
