During the COVID-19 lockdown period (from January 23 to February 29, 2020), ambient PM 2.5 concentrations in the Yangtze River Delta (YRD) region were observed to be much lower, while the maximum daily 8 h average (MDA8) O 3 concentrations became much higher compared to those before the lockdown (from January 1 to 22, 2020). Here, we show that emission reduction is the major driving force for the PM 2.5 change, contributing to a PM 2.5 decrease by 37% to 55% in the four YRD major cities (i.e., Shanghai, Hangzhou, Nanjing, and Hefei), but the MDA8 O 3 increase is driven by both emission reduction (29%–52%) and variation in meteorological conditions (17%– 49%). Among all pollutants, reduction in emissions mainly of primary PM contributes to a PM 2.5 decrease by 28% to 46%, and NOx emission reduction contributes 7% to 10%. Although NOx emission reduction dominates the MDA8 O 3 increase (38%–59%), volatile organic compounds (VOCs) emission reduction lead to a 5% to 9% MDA8 O 3 decrease. Increased O 3 promotes secondary aerosol formation and partially offsets the decrease of PM 2.5 caused by the primary PM emission reductions. The results demonstrate that more coordinated air pollution control strategies are needed in YRD.

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Abstract. A high-resolution air pollutant emission inventory for the Yangtze River Delta (YRD) region was updated for 2017 using emission factors and chemical speciation based mainly on local measurements in this study. The inventory included 424 non-methane volatile organic compounds (NMVOCs) and 43 fine particulate matter (PM2.5) species from 259 specific sources. The total emissions of SO2, NOx, CO, NMVOCs, PM10, PM2.5, and NH3 in the YRD region in 2017 were 1552, 3235, 38 507, 4875, 3770, 1597, and 2467 Gg, respectively. SO2 and CO emissions were mainly from boilers, accounting for 49 % and 73 % of the total. Mobile sources dominated NOx emissions, contributing 57 % of the total. NMVOC emissions, mainly from industrial sources, made up 61 % of the total. Dust sources accounted for 55 % and 28 % of PM10 and PM2.5 emissions, respectively. Agricultural sources accounted for 91 % of NH3 emissions. Major PM2.5 species were OC, Ca, Si, PSO4, and EC, accounting for 9.0 %, 7.0 %, 6.4 %, 4.6 %, and 4.3 % of total PM2.5 emissions, respectively. The main species of NMVOCs were aromatic hydrocarbons, making up 25.3 % of the total. Oxygenated volatile organic compounds (OVOCs) contributed 21.9 % of the total NMVOC emissions. Toluene had the highest comprehensive contribution to ozone (O3) and secondary organic aerosol (SOA) formation potentials, while other NMVOCs included 1,2,4-trimethylbenzene, m,p-xylene, propylene, ethene, o-xylene, and ethylbenzene. Industrial process and solvent-use sources were the main sources of O3 and SOA formation potential, followed by motor vehicles. Among industrial sources, chemical manufacturing, rubber and plastic manufacturing, appliance manufacturing, and textiles made significant contributions. This emission inventory should provide scientific guidance for future control of air pollutants in the YRD region of China.

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Abstract. Rapid sulfate formation is recognized as a key characteristic of severe winter haze in China. However, air quality models tend to underestimate sulfate formation during heavy haze periods, and heterogeneous formation pathways have been proposed as promising mechanisms to reduce gaps between observation and model simulation. In this study, we implemented a reactive SO2 uptake mechanism through the SO2+NO2 heterogeneous reactions in the Comprehensive Air Quality Model with Extensions (CAMx) to improve simulation of sulfate formation in the Yangtze River Delta (YRD) region. Parameterization of the SO2+NO2 heterogeneous reactions is based on observations in Beijing and considered both the impact of relative humidity and aerosol pH on sulfate formation. Ammonia is reported to be critical for the formation of secondary inorganic aerosols. Estimation of ammonia emissions is usually associated with large uncertainties and models tend to underestimate ammonia concentrations substantially. Sensitivity tests were conducted to evaluate the influence of the SO2+NO2 heterogeneous reactions as well as ammonia emissions on modeled sulfate concentrations during a period with several heavy haze episodes in the YRD region. Base case model results show large underestimation of sulfate concentrations by 36 % under polluted conditions in the YRD region. Adding the SO2+NO2 heterogeneous reactions or doubling ammonia emissions alone leads to slight model improvement (∼6 %) on simulated sulfate concentrations in the YRD region. However, model performance significantly improved when both the SO2+NO2 heterogeneous reactions and doubled ammonia emissions were included in the simulation: predicted sulfate concentrations during polluted periods increased from 23.1 µg m−3 in the base scenario to 29.1 µg m−3 (representing an increase of 26 %). Aerosol pH is crucial for the SO2+NO2 heterogeneous reactions, and our calculated aerosol pH is always acidic and increased by 0.7 with doubled ammonia emissions. Modeling results also show that this reactive SO2 uptake mechanism enhanced sulfate simulations by 1 to 5 µg m−3 for the majority of the eastern and central parts of China, with more than 20 µg m−3 increase in sulfate concentrations over the northeastern plain. These findings suggest that the SO2+NO2 heterogeneous reactions could be potentially important for sulfate formation in the YRD region as well as other parts of China. Further studies are needed to constrain the uncertainties associated with the parameterization of the SO2+NO2 heterogeneous reactions based on local data as well as to evaluate this mechanism in other regions. In addition, ammonia emissions were found to be a key driving variable of the spatial patterns of sulfate enhancement due to the new pathway. Substantial efforts are needed to improve the accuracy of the ammonia emission inventory.