Unbalanced emission reductions of different species and sectors in China during COVID-19 lockdown derived by multi-species surface observation assimilation

The unprecedented lockdown of human activities during the COVID-19 pandemic has significantly influenced social life in China. However, understanding the impact of this unique event on the emissions of different species is still insufficient, prohibiting the proper assessment of the environmental impacts of COVID-19 restrictions. Here we developed a multi-air-pollutant inversion system to simultaneously estimate the emissions of NOx, SO2, CO, PM2.5 and PM10 in China during COVID-19 restrictions with high temporal (daily) and horizontal (15 km) resolutions. Subsequently, contributions of emission changes versus meteorological variations during the COVID-19 lockdown were separated and quantified. The results demonstrated that the inversion system effectively reproduced the actual emission variations in multi-air pollutants in China during different periods of COVID-19 lockdown, which indicate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing substantially by ∼40 %. However, emissions of other air pollutants were found to only decrease by∼10% because power generation and heavy industrial processes were not halted during lockdown, and residential activities may actually have increased due to the stay-at-home orders. Consequently, although obvious reductions of PM2.5 concentrations occurred over the North China Plain (NCP) during the lockdown period, the emission change only accounted for 8.6 % of PM2.5 reductions and even led to substantial increases in O3. The meteorological variation instead dominated the changes in PM2.5 concentrations over the NCP, which contributed 90 % of the PM2.5 reductions over most parts of the NCP region. Meanwhile, our results suggest that the local stagnant meteorological conditions, together with inefficient reductions of PM2.5 emissions, were the main drivers of the unexpected PM2.5 pollution in Beijing during the lockdown period. These results highlighted that traffic control as a separate pollution control measure has limited effects on the coordinated control of O3 and PM2.5 concentrations under current complex air pollution conditions in China. More comprehensive and balanced regulations for multiple precursors from different sectors are required to address O3 and PM2.5 pollution in China.

Coarse particulate matter air quality in East Asia: implications for fine particulate nitrate

Air quality network data in China and South Korea show very high year-round mass concentrations of coarse particulate matter (PM), as inferred by the difference between PM10 and PM2.5. Coarse PM concentrations in 2015 averaged 52 µg m-3 in the North China Plain (NCP) and 23 µg m-3 in the Seoul Metropolitan Area (SMA), contributing nearly half of PM10. Strong daily correlations between coarse PM and carbon monoxide imply a dominant source from anthropogenic fugitive dust. Coarse PM concentrations in the NCP and the SMA decreased by 21 % from 2015 to 2019 and further dropped abruptly in 2020 due to COVID-19 reductions in construction and vehicle traffic. Anthropogenic coarse PM is generally not included in air quality models but scavenges nitric acid to suppress the formation of fine particulate nitrate, a major contributor to PM2.5 pollution. GEOS-Chem model simulation of surface and aircraft observations from the Korea–United States Air Quality (KORUS-AQ) campaign over the SMA in May–June 2016 shows that consideration of anthropogenic coarse PM largely resolves the previous model overestimate of fine particulate nitrate. The effect is smaller in the NCP which has a larger excess of ammonia. Model sensitivity simulations for 2015–2019 show that decreasing anthropogenic coarse PM directly increases PM2.5 nitrate in summer, offsetting 80 % the effect of nitrogen oxide and ammonia emission controls, while in winter the presence of coarse PM increases the sensitivity of PM2.5 nitrate to ammonia and sulfur dioxide emissions. Decreasing coarse PM helps to explain the lack of decrease in wintertime PM2.5 nitrate observed in the NCP and the SMA over the 2015–2021 period despite decreases in nitrogen oxide and ammonia emissions. Continuing decrease of fugitive dust pollution means that more stringent nitrogen oxide and ammonia emission controls will be required to successfully decrease PM2.5 nitrate.

Separating Daily 1 km PM2.5 Inorganic Chemical Composition in China since 2000 via Deep Learning Integrating Ground, Satellite, and Model Data.

Fine particulate matter (PM2.5) chemical composition has strong and diverse impacts on the planetary environment, climate, and health. These effects are still not well understood due to limited surface observations and uncertainties in chemical model simulations. We developed a four-dimensional spatiotemporal deep forest (4D-STDF) model to estimate daily PM2.5 chemical composition at a spatial resolution of 1 km in China since 2000 by integrating measurements of PM2.5 species from a high-density observation network, satellite PM2.5 retrievals, atmospheric reanalyses, and model simulations. Cross-validation results illustrate the reliability of sulfate (SO42-), nitrate (NO3-), ammonium (NH4+), and chloride (Cl-) estimates, with high coefficients of determination (CV-R2) with ground-based observations of 0.74, 0.75, 0.71, and 0.66, and average root-mean-square errors (RMSE) of 6.0, 6.6, 4.3, and 2.3 µg/m3, respectively. The three components of secondary inorganic aerosols (SIAs) account for 21% (SO42-), 20% (NO3-), and 14% (NH4+) of the total PM2.5 mass in eastern China; we observed significant reductions in the mass of inorganic components by 40-43% between 2013 and 2020, slowing down since 2018. Comparatively, the ratio of SIA to PM2.5 increased by 7% across eastern China except in Beijing and nearby areas, accelerating in recent years. SO42- has been the dominant SIA component in eastern China, although it was surpassed by NO3- in some areas, e.g., Beijing-Tianjin-Hebei region since 2016. SIA, accounting for nearly half (∼46%) of the PM2.5 mass, drove the explosive formation of winter haze episodes in the North China Plain. A sharp decline in SIA concentrations and an increase in SIA-to-PM2.5 ratios during the COVID-19 lockdown were also revealed, reflecting the enhanced atmospheric oxidation capacity and formation of secondary particles.

Radiative effects and feedbacks of anthropogenic aerosols on boundary layer meteorology and fine particulate matter during the COVID-19 lockdown over China.

The COVID-19 epidemic has exerted significant impacts on human health, social and economic activities, air quality and atmospheric chemistry, and potentially on climate change. In this study, an online coupled regional climate-chemistry-aerosol model (RIEMS-Chem) was applied to explore the direct, indirect, and feedback effects of anthropogenic aerosols on radiation, boundary layer meteorology, and fine particulate matter during the COVID-19 lockdown period from 23 January to 8 April 2020 over China. Model performance was validated against a variety of observations for meteorological variables, PM2.5 and its chemical components, aerosol optical properties, as well as shortwave radiation flux, which demonstrated that RIEMS-Chem was able to reproduce the spatial distribution and temporal variation of the above variables reasonably well. During the study period, direct radiative effect (DRE) of anthropogenic aerosols was stronger than indirect radiative effect (IRE) in most regions north of the Yangtze River, whereas IRE dominated over DRE in the Yangtze River regions and South China. In North China, DRE induced larger changes in meteorology and PM2.5 than those induced by IRE, whereas in South China, the changes by IRE were remarkably larger than those by DRE. Emission reduction alone during the COVID-19 lockdown reduced PM2.5 concentration by approximately 32 % on average over East China. As a result, DRE at the surface was weakened by 15 %, whereas IRE changed little over East China, leading to a decrease in total radiative effect (TRE) by approximately 7 % in terms of domain average. The DRE-induced changes in meteorology and PM2.5 were weakened due to emission reduction, whereas the IRE-induced changes were almost the same between the cases with and without emission reductions. By aerosol radiative and feedback effects, the COVID-19 emission reductions resulted in 0.06 °C and 0.04 °C surface warming, 1.6 and 4.0 µg m-3 PM2.5 decrease, 0.4 and 1.3 mm precipitation increase during the lockdown period in 2020 in terms of domain average over North China and South China, respectively, whereas the lockdown caused negligible changes on average over East Asia.

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.

The effect of COVID-19 restrictions on atmospheric new particle formation in Beijing

During the COVID-19 lockdown, the dramatic reduction of anthropogenic emissions provided a unique opportunity to investigate the effects of reduced anthropogenic activity and primary emissions on atmospheric chemical processes and the consequent formation of secondary pollutants. Here, we utilize comprehensive observations to examine the response of atmospheric new particle formation (NPF) to the changes in the atmospheric chemical cocktail. We find that the main clustering process was unaffected by the drastically reduced traffic emissions, and the formation rate of 1.5 nm particles remained unaltered. However, particle survival probability was enhanced due to an increased particle growth rate (GR) during the lockdown period, explaining the enhanced NPF activity in earlier studies. For GR at 1.5–3 nm, sulfuric acid (SA) was the main contributor at high temperatures, whilst there were unaccounted contributing vapors at low temperatures. For GR at 3–7 and 7–15 nm, oxygenated organic molecules (OOMs) played a major role. Surprisingly, OOM composition and volatility were insensitive to the large change of atmospheric NOx concentration;instead the associated high particle growth rates and high OOM concentration during the lockdown period were mostly caused by the enhanced atmospheric oxidative capacity. Overall, our findings suggest a limited role of traffic emissions in NPF.

Impact of Chemical Properties of Human Respiratory Droplets and Aerosol Particles on Airborne Viruses' Viability and Indoor Transmission.

The airborne transmission of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) has been identified as a potential pandemic challenge, especially in poorly ventilated indoor environments, such as certain hospitals, schools, public buildings, and transports. The impacts of meteorological parameters (temperature and humidity) and physical property (droplet size) on the airborne transmission of coronavirus in indoor settings have been previously investigated. However, the impacts of chemical properties of viral droplets and aerosol particles (i.e., chemical composition and acidity (pH)) on viability and indoor transmission of coronavirus remain largely unknown. Recent studies suggest high organic content (proteins) in viral droplets and aerosol particles supports prolonged survival of the virus by forming a glassy gel-type structure that restricts the virus inactivation process under low relative humidity (RH). In addition, the virus survival was found at neutral pH, and inactivation was observed to be best at low (<5) and high pH (>10) values (enveloped bacteriophage Phi6). Due to limited available information, this article illustrates an urgent need to research the impact of chemical properties of exhaled viral particles on virus viability. This will improve our fundamental understanding of indoor viral airborne transmission mechanisms.

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.

Nitrate and secondary organic aerosol dominated particle light extinction in Beijing due to clean air action

Air quality in China has been continuously improved since clean air action in 2013, yet the visibility was not improved simultaneously. Here we employed a new method by integrating highly-time resolved aerosol compositions with particle light extinction (bext) into positive matrix factorization to quantify the different contributors to visibility degradation during four seasons in Beijing. Our results show that ammonium nitrate-related factor contributed dominantly to bext during all seasons (31–48%) and played more significant roles during low-visibility periods. Secondary organic aerosol (SOA) was an important contributor of bext (27–35%) in autumn and spring while primary OA related sources were more important in winter (37%). An increase in aerosol mass extinction efficiency and similarly important roles of ammonium nitrate and SOA in visibility degradation were also observed during COVID-19 lockdown. Our results point towards a future challenge in improving visibility in China due to the increased contributions of nitrate and SOA in PM2.5. Future emission controls with a priority to decrease nitrate would benefit both air quality and visibility.

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.