Abstract

Due to the nonlinear impacts of meteorology and precursors, the response of ozone (O3) trends to emission changes is very complex over different regions in megacity Beijing. Based on long-term in-situ observations at 35 air quality sites (four categories, i.e., urban, traffic, northern suburban and southern suburban sites) and satellite data, spatiotemporal variability of O3, gaseous precursors, and O3-VOCs-NOx sensitivity were explored through multiple metrics during the warm season from 2013 to 2020. Additionally, the contribution of meteorology and emissions to O3 was separated by a machine-learning-based de-weathered method. The annual averaged MDA8 O3 and O3 increased by 3.7 and 2.9 μg/m3/yr, respectively, with the highest at traffic sites and the lowest in northern suburb, and the rate of Ox (O3 + NO2) was 0.2 μg/m3/yr with the highest in southern suburb, although NO2 declined strongly and HCHO decreased slightly. However, the increment of O3 and Ox in the daytime exhibited decreasing trends to some extent. Additionally, NOx abatements weakened O3 loss through less NO titration, which drove narrowing differences in urban-suburban O3 and Ox. Due to larger decrease of NO2 in urban region and HCHO in northern suburb, the extent of VOCs-limited regime fluctuated over Beijing and northern suburb gradually shifted to transition or NOx-limited regime. Compared with the directly observed trends, the increasing rate of de-weathered O3 was lower, which was attributed to favorable meteorological conditions for O3 generation after 2017, especially in June (the most polluted month); whereas the de-weathered Ox declined except in southern suburb. Overall, clean air actions were effective in reducing the atmospheric oxidation capacity in urban and northern suburban regions, weakening local photochemical production over Beijing and suppressing O3 deterioration in northern suburb. Strengthening VOCs control and keeping NOx abatement, especially in June, will be vital to reverse O3 increase trend in Beijing.

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