Changes in primary and secondary aerosols during a controlled Chinese New Year.

Large reductions in anthropogenic emissions during the Chinese New Year (CNY) holiday in Beijing have been well reported. However, the changes during the CNY of 2021 are different because most people stayed in Beijing to control the spread of coronavirus disease (COVID-19). Here a high-resolution aerosol mass spectrometer (HR-AMS) was deployed for characterization of the changes in size-resolved aerosol composition and sources during the CNY. We found that the reductions in traffic-related NOx and fossil fuel-related organic aerosol (OA), and cooking OA (1.3-12.7%) during the CNY of 2021 were much smaller than those in previous CNY holidays of 2013, 2015, and 2020. In contrast, the mass concentrations of secondary aerosol species except nitrate showed ubiquitous increases (17.6-30.4%) during the CNY of 2021 mainly due to a 4-day severe haze episode. OA composition also changed substantially during the CNY of 2021. In particular, we observed a large increase by nearly a factor of 2 in oxidized primary OA likely from biomass burning, and a decrease of 50.1% in aqueous-phase secondary OA. A further analysis of the severe haze episode during the CNY illustrated a rapid transition of secondary formation from photochemical to aqueous-phase processing followed by a scavenging process, leading to significant changes in aerosol composition, size distributions, and oxidation degree of OA. A parameterization relationship between oxygen-to-carbon (O/C) and f44 (fraction of m/z 44 in OA) from a collocated capture vaporizer aerosol chemical speciation monitor (CV-ACSM) was developed, which has a significant implication for characterization of OA evolution and the impacts on hygroscopicity due to the rapidly increased deployments of CV-ACSM worldwide.

Machine learning elucidates the impact of short-term emission changes on air pollution in Beijing

The Chinese Spring Festival (CSF) is the most solemn traditional festival in China, and the substantial changes in anthropogenic activities in megacities provide a unique natural experiment to assess the influence of short-term emission changes on air quality. Here we applied a machine learning based random forest algorithm to six-year aerosol composition measurements in urban Beijing during the CSFs of 2012–2020 to quantify the relative contributions of meteorology and emission changes to air quality. Our results demonstrate large variabilities of air pollutants during the CSF due to the meteorological changes and holiday effect. By removing the meteorological effect, we found that the reduced emissions during CSF caused an average decrease of 5.1% for non-refractory PM2.5 with chloride and primary organic aerosol being the largest (8.8–18.7%) while the changes in secondary species were small. The COVID-19 lockdown during 2020 led to additional reductions of primary species by 16.3–36.8%, yet increases in nitrate and secondary organic aerosol due to enhanced secondary production. Our study has a significant implication that reducing local traffic and cooking emissions is far from enough for mitigating air pollution in winter in megacities due to the nonlinear effect of secondary production and regional transport. A synergetic control of multiple precursors, e.g., NOx and ammonia, is of great importance to reduce secondary aerosol and improve air quality.

A chemical cocktail during the COVID-19 outbreak in Beijing, China: Insights from six-year aerosol particle composition measurements during the Chinese New Year holiday.

The rapidly spread coronavirus disease (COVID-19) has limited people's outdoor activities and hence caused substantial reductions in anthropogenic emissions around the world. However, the air quality in some megacities has not been improved as expected due to the complex responses of aerosol chemistry to the changes in precursors and meteorology. Here we demonstrate the responses of primary and secondary aerosol species to the changes in anthropogenic emissions during the COVID-19 outbreak in Beijing, China along with the Chinese New Year (CNY) holiday effects on air pollution by using six-year aerosol particle composition measurements. Our results showed large reductions in primary aerosol species associated with traffic, cooking and coal combustion emissions by 30-50% on average during the CNY, while the decreases in secondary aerosol species were much small (5-12%). These results point towards a future challenge in mitigating secondary air pollution because the reduced gaseous precursors may not suppress secondary aerosol formation efficiently under stagnant meteorological conditions. By analyzing the long-term measurements from 2012 to 2020, we found considerable increases in the ratios of nitrate to sulfate, secondary to primary OA, and sulfur and nitrogen oxidation capacity despite the overall decreasing trends in mass concentrations of most aerosol species, suggesting that the decreases in anthropogenic emissions have facilitated secondary formation processes during the last decade. Therefore, a better understanding of the mechanisms driving the chemical responses of secondary aerosol to the changes in anthropogenic emissions under complex meteorological environment is essential for future mitigation of air pollution in China.