ABSTRACT
Organic aerosol (OA) is a major component of atmospheric particulate matter (PM) with complex composition and formation processes influenced by various factors. Emission reduction can alter both precursors and oxidants which further affects secondary OA formation. Here we provide an observational analysis of secondary OA (SOA) variation properties in Yangtze River Delta (YRD) of eastern China in response to large scale of emission reduction during Chinese New Year (CNY) holidays from 2015 to 2020, and the COVID-19 pandemic period from January to March, 2020. We found a 17% increase of SOA proportion during the COVID lockdown. The relative enrichment of SOA is also found during multi-year CNY holidays with dramatic reduction of anthropogenic emissions. Two types of oxygenated OA (OOA) influenced by mixed emissions and SOA formation were found to be the dominant components during the lockdown in YRD region. Our results highlight that these emission-reduction-induced changes in organic aerosol need to be considered in the future to optimize air pollution control measures. Electronic Supplementary Material: Supplementary material is available in the online version of this article at 10.1007/s11783-023-1714-0 and is accessible for authorized users.
ABSTRACT
By using WRF-Chem coupled with a heterogeneous reaction mechanism for sulfate formation, this study investigated the impact of meteorological condition and emission changes on chemical species, atmospheric oxidizing capacity (AOC), and secondary aerosol formation during the COVID-19 lockdown period from 23 January to April 8, 2020, focusing on a severe haze event on 7-14 February. The model with the new sulfate formation scheme reasonably reproduces the spatial-temporal distribution of meteorological variables and chemical species, and significantly improves predictions for both sulfate and SO2 concentrations, as well as for PM2.5, ammonium, and nitrate to some extent. It is found that the adverse meteorological conditions were the main cause for the haze event formation, whereas emission reduction due to the lockdown somewhat decreased PM2.5 concentration on average in the Beijing-Tianjin-Hebei (BTH) region. Compared with the same period in 2019, increased surface air temperature and relative humidity (RH) and decreased planetary boundary layer height (PBLH) facilitated accumulation of pollutants and formation of secondary aerosols during the haze episode in 2020, whereas the emission reduction due to the lockdown led to decreases in SO2, NO2, primary PM2.5 (PPM2.5), black carbon (BC), primary organic aerosols (POA), nitrate and ammonium concentrations, but increases in O3, sulfate and secondary organic aerosol (SOA) concentrations, due to the combined effect of changes in emissions and AOC. Gas and aqueous phase oxidation of SO2 accounted for approximately 24% of sulfate formation, while the heterogeneous reaction of Mn-catalytic oxidation of SO2 on aerosol surfaces dominated sulfate formation (76%) during the haze episode in the BTH region. Both adverse meteorological conditions and emission reductions increased heterogeneous sulfate formation rate mainly through altering aerosol surface area (ASA), pH, and Mn2+ concentration. Chemical species varied diversely during the three subperiods before (Period-1, 15-22 January) and during the lockdown (Period-2, 23 January to 5 March and Period-3, 6 March to 8 April) over the BTH. NO2 concentration firstly decreased and then rebounded, whereas O3 concentration increased gradually from the Period-1 to Period-3. All aerosols except SOA decreased throughout the lockdown period, whereas SOA peaked in the Period-2 due to its strong sensitivity to increasing AOC. Sulfate concentration decreased from the Period-1 to Period-2, mainly due to more adverse meteorological conditions in the Period-1, although sulfate increased slightly due to increasing AOC in the Period-2. The large difference in the direction and magnitude of species variations during the COVID-19 lockdown indicates the complex interplay among meteorology, emission, and chemistry. Copyright © 2022 Elsevier Ltd
ABSTRACT
Nationwide restrictions on human activities (lockdown) in China since 23 January 2020, to control the 2019 novel coronavirus disease pandemic (COVID-19), has provided an opportunity to evaluate the effect of emission mitigation on particulate matter (PM) pollution. The WRF-Chem simulations of persistent heavy PM pollution episodes from 20 January to 14 February 2020, in the Guanzhong Basin (GZB), northwest China, reveal that large-scale emission reduction of primary pollutants has not substantially improved the air quality during the COVID-19 lockdown period. Simultaneous reduction of primary precursors during the lockdown period only decreases the near-surface PM2.5 mass concentration by 11.6% (12.6 µg m-3), but increases ozone (O3) concentration by 9.2% (5.5 µg m-3) in the GZB. The primary organic aerosol and nitrate are the major contributor to the decreased PM2.5 in the GZB, with the reduction of 28.0% and 21.8%, respectively, followed by EC (10.1%) and ammonium (7.2%). The increased atmospheric oxidizing capacity by the O3 enhancement facilitates the secondary aerosol (SA) formation in the GZB, increasing secondary organic aerosol and sulphate by 6.5% and 3.3%, respectively. Furthermore, sensitivity experiments suggest that combined emission reduction of NOX and VOCs following the ratio of 1:1 is conducive to lowering the wintertime SA and O3 concentration and further alleviating the PM pollution in the GZB.
ABSTRACT
To control the spread of COVID-19, China implemented a series of lockdowns, limiting various offline interactions. This provided an opportunity to study the response of air quality to emissions control. By comparing the characteristics of pollution in the summers of 2019 and 2020, we found a significant decrease in gaseous pollutants in 2020. However, particle pollution in the summer of 2020 was more severe; PM2.5 levels increased from 35.8 to 44.7 µg m-3, and PM10 increased from 51.4 to 69.0 µg m-3 from 2019 to 2020. The higher PM10 was caused by two sandstorm events on May 11 and June 3, 2020, while the higher PM2.5 was the result of enhanced secondary formation processes indicated by the higher sulfate oxidation rate (SOR) and nitrate oxidation rate (NOR) in 2020. Higher SOR and NOR were attributed mainly to higher relative humidity and stronger oxidizing capacity. Analysis of PMx distribution showed that severe haze occurred when particles within Bin2 (size ranging 1-2.5 µm) dominated. SO42-(1/2.5) and SO42-(2.5/10) remained stable under different periods at 0.5 and 0.8, respectively, indicating that SO42- existed mainly in smaller particles. Decreases in NO3-(1/2.5) and increases in NO3-(2.5/10) from clean to polluted conditions, similar to the variations in PMx distribution, suggest that NO3- played a role in the worsening of pollution. O3 concentrations were higher in 2020 (108.6 µg m-3) than in 2019 (96.8 µg m-3). Marked decreases in fresh NO alleviated the titration of O3. Furthermore, the oxidation reaction of NO2 that produces NO3- was dominant over the photochemical reaction of NO2 that produces O3, making NO2 less important for O3 pollution. In comparison, a lower VOC/NOx ratio (less than 10) meant that Beijing is a VOC-limited area; this indicates that in order to alleviate O3 pollution in Beijing, emissions of VOCs should be controlled.