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Abstract. 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 in NOx emissions. NOx emission reductions lead to increases in O3 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.

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/m 3 . 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/m 3 . 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/m 3 , 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.