Drivers of High Concentrations of Secondary Organic Aerosols in Northern China during the COVID-19 Lockdowns.

During the COVID-19 lockdown in early 2020, observations in Beijing indicate that secondary organic aerosol (SOA) concentrations increased despite substantial emission reduction, but the reasons are not fully explained. Here, we integrate the two-dimensional volatility basis set into a state-of-the-art chemical transport model, which unprecedentedly reproduces organic aerosol (OA) components resolved by the positive matrix factorization based on aerosol mass spectrometer observations. The model shows that, for Beijing, the emission reduction during the lockdown lowered primary organic aerosol (POA)/SOA concentrations by 50%/18%, while deteriorated meteorological conditions increased them by 30%/119%, resulting in a net decrease in the POA concentration and a net increase in the SOA concentration. Emission reduction and meteorological changes both led to an increased OH concentration, which accounts for their distinct effects on POA and SOA. SOA from anthropogenic volatile organic compounds and organics with lower volatility contributed 28 and 62%, respectively, to the net SOA increase. Different from Beijing, the SOA concentration decreased in southern Hebei during the lockdown because of more favorable meteorology. Our findings confirm the effectiveness of organic emission reductions and meanwhile reveal the challenge in controlling SOA pollution that calls for large organic precursor emission reductions to rival the adverse impact of OH increase.

Ambient fine particulate matter and ozone pollution in China: synergy in anthropogenic emissions and atmospheric processes

Since 2013, China has taken a series of actions to relieve serious PM2.5 pollution. As a result, the annual PM2.5 concentration decreased by more than 50% from 2013 to 2021. However, ozone pollution has become more pronounced, especially in the North China Plain. Here, we review the impacts of anthropogenic emissions, meteorology, and atmospheric processes on ambient PM2.5 loading and components and O3 pollution in China. The reported influence of interannual meteorological changes on PM2.5 and O3 pollution during 2013–2019 ranged from 10%–20% and 20%–40%, respectively. During the same period, the anthropogenic emissions of NOx, SO2, primary PM2.5, NMVOC and NH3 are estimated to decrease by 38%, 51%, 35%, 11% and 17%, respectively. Such emission reduction is the main cause for the decrease in PM2.5 concentration across China. However, the imbalanced reductions in various precursors also result in the variation in nitrate gas-particle partitioning and hence an increase in the nitrate fraction in PM2.5. The increase of ozone concentration and the enhancement of atmospheric oxidation capacity can also have substantial impact on the secondary components of PM2.5, which partly explained the growth of organic aerosols during haze events and the COVID-19 shutdown period. The uneven reduction in NOx and NMVOC is suggested to be the most important reason for the rapid O3 increase after 2013. In addition, the decrease in PM2.5 may also have affected O3 formation via radiation effects and heterogeneous reactions. Moreover, climate change is expected to influence both anthropogenic emissions and atmospheric processes. However, the extent and pathways of the PM2.5-O3 interplay and how it will be impacted by the changing emission and atmospheric conditions making the synergetic control of PM2.5 and O3 difficult. Further research on the interaction of PM2.5 and O3 is needed to provide basis for a scientifically-grounded and effective co-control strategy.

Variations and Sources of Organic Aerosol in Winter Beijing under Markedly Reduced Anthropogenic Activities During COVID-2019.

The COVID-19 outbreak provides a "controlled experiment" to investigate the response of aerosol pollution to the reduction of anthropogenic activities. Here we explore the chemical characteristics, variations, and emission sources of organic aerosol (OA) based on the observation of air pollutants and combination of aerosol mass spectrometer (AMS) and positive matrix factorization (PMF) analysis in Beijing in early 2020. By eliminating the impacts of atmospheric boundary layer and the Spring Festival, we found that the lockdown effectively reduced cooking-related OA (COA) but influenced fossil fuel combustion OA (FFOA) very little. In contrast, both secondary OA (SOA) and O3 formation was enhanced significantly after lockdown: less-oxidized oxygenated OA (LO-OOA, 37% in OA) was probably an aged product from fossil fuel and biomass burning emission with aqueous chemistry being an important formation pathway, while more-oxidized oxygenated OA (MO-OOA, 41% in OA) was affected by regional transport of air pollutants and related with both aqueous and photochemical processes. Combining FFOA and LO-OOA, more than 50% of OA pollution was attributed to combustion activities during the whole observation period. Our findings highlight that fossil fuel/biomass combustion are still the largest sources of OA pollution, and only controlling traffic and cooking emissions cannot efficiently eliminate the heavy air pollution in winter Beijing.

Non-negligible contributions to human health from increased household air pollution exposure during the COVID-19 lockdown in China.

BACKGROUND: Ambient and household air pollution are found to lead to premature deaths from all-cause or cause-specific death. The national lockdown measures in China during COVID-19 were found to lead to abrupt changes in ambient surface air quality, but indoor air quality changes were neglected. In this study, we aim to investigate the impacts of lockdown measures on both ambient and household air pollution as well as the short-term health effects of air pollution changes. METHODS: In this study, an up-to-date emission inventory from January to March 2020 in China was developed based on air quality observations in combination with emission-concentration response functions derived from chemical transport modeling. These emission inventories, together with the emissions data from 2017 to 2019, were fed into the state-of-the-art regional chemistry transport model to simulate the air quality in the North China Plain. A hypothetical scenario assuming no lockdown effects in 2020 was also performed to determine the effects of the lockdown on air quality in 2020. A difference-to-difference approach was adopted to isolate the effects on air quality due to meteorological conditions and long-term decreasing emission trends by comparing the PM2.5 changes during lockdown to those before lockdown in 2020 and in previous years (2017-2019). The short-term premature mortality changes from both ambient and household PM2.5 changes were quantified based on two recent epidemiological studies, with uncertainty of urban and rural population migration considerations. FINDINGS: The national lockdown measures during COVID-19 led to a reduction of 5.1 µg m-3 in ambient PM2.5 across the North China Plain (NCP) from January 25th to March 5th compared with the hypothetical simulation with no lockdown measures. However, a difference-to-difference method showed that the daily domain average PM2.5 in the NCP decreased by 9.7 µg m-3 between lockdown periods before lockdown in 2020, while it decreased by 7.9 µg m-3 during the same periods for the previous three-year average from 2017 to 2019, demonstrating that lockdown measures may only have caused a 1.8 µg m-3 decrease in the NCP. We then found that the integrated population-weighted PM2.5, including both ambient and indoor PM2.5 exposure, increased by 5.1 µg m-3 during the lockdown periods compared to the hypothetical scenario, leading to additional premature deaths of 609 (95% CI: 415-775) to 2,860 (95% CI: 1,436-4,273) in the short term, depending on the relative risk chosen from the epidemiological studies. INTERPRETATION: Our study indicates that lockdown measures in China led to abrupt reductions in ambient PM2.5 concentration but also led to significant increases in indoor PM2.5 exposure due to confined indoor activities and increased usages of household fuel for cooking and heating. We estimated that hundreds of premature deaths were added as a combination of decreased ambient PM2.5 and increased household PM2.5. Our findings suggest that the reduction in ambient PM2.5 was negated by increased exposure to household air pollution, resulting in an overall increase in integrated population weighted exposure. Although lockdown measures were instrumental in reducing the exposure to pollution concentration in cities, rural areas bore the brunt, mainly due to the use of dirty solid fuels, increased population density due to the large-scale migration of people from urban to rural areas during the Chinese New Year and long exposure time to HAP due to restrictions in outdoor movement.

Quantifying the emission changes and associated air quality impacts during the COVID-19 pandemic on the North China Plain: a response modeling study

Quantification of emission changes is a prerequisite for the assessment of control effectiveness in improving air quality. However, the traditional bottom-up method for characterizing emissions requires detailed investigation of emissions data (e.g., activity and other emission parameters) that usually takes months to perform and limits timely assessments. Here we propose a novel method to address this issue by using a response model that provides real-time estimation of emission changes based on air quality observations in combination with emission-concentration response functions derived from chemical transport modeling. We applied the new method to quantify the emission changes on the North China Plain (NCP) due to the COVID-19 pandemic shutdown, which overlapped the Spring Festival (also known as Chinese New Year) holiday. Results suggest that the anthropogenic emissions of NO2,SO2, volatile organic compound (VOC) and primary PM2.5 on the NCP were reduced by 51 %, 28 %, 67 % and 63 %, respectively, due to the COVID-19 shutdown, indicating longer and stronger shutdown effects in 2020 compared to the previous Spring Festival holiday. The reductions of VOC and primary PM2.5 emissions are generally effective in reducing O3 and PM2.5 concentrations. However, such air quality improvements are largely offset by reductions inNOx emissions. NOx emission reductions lead to increases inO3 and PM2.5 concentrations on the NCP due to the strongly VOC-limited conditions in winter. A strong NH3-rich condition is also suggested from the air quality response to the substantial NOx emission reduction. Well-designed control strategies are recommended based on the air quality response associated with the unexpected emission changes during the COVID-19 period. In addition, our results demonstrate that the new response-based inversion model can well capture emission changes based on variations in ambient concentrations and thereby illustrate the great potential for improving the accuracy and efficiency of bottom-up emission inventory methods.

Impact of emission reductions and meteorology changes on atmospheric mercury concentrations during the COVID-19 lockdown.

Controlling anthropogenic mercury emissions is an ongoing effort and the effect of atmospheric mercury mitigation is expected to be impacted by accelerating climate change. The lockdown measures to restrict the spread of Coronavirus Disease 2019 (COVID-19) and the following unfavorable meteorology in Beijing provided a natural experiment to examine how air mercury responds to strict control measures when the climate becomes humid and warm. Based on a high-time resolution emission inventory and generalized additive model, we found that air mercury concentration responded almost linearly to the changes in mercury emissions when excluding the impact of other factors. Existing pollution control and additional lockdown measures reduced mercury emissions by 16.7 and 12.5 kg/d during lockdown, respectively, which correspondingly reduced the concentrations of atmospheric mercury by 0.10 and 0.07 ng/m3. Emission reductions from cement clinker production contributed to the largest decrease in atmospheric mercury, implying potential mitigation effects in this sector since it is currently the number one emitter in China. However, changes in meteorology raised atmospheric mercury by 0.41 ng/m3. The increases in relative humidity (9.5%) and temperature (1.2 °C) significantly offset the effect of emission reduction by 0.17 and 0.09 ng/m3, respectively, which highlights the challenge of air mercury control in humid and warm weather and the significance of understanding mercury behavior in the atmosphere and at atmospheric interfaces, especially the impact from relative humidity.