Satellite-Based Diagnosis and Numerical Verification of Ozone Formation Regimes over Nine Megacities in East Asia

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Abstract
Urban photochemical ozone (O3) formation regimes (NOx- and VOC-limited regimes) at nine megacities in East Asia were diagnosed based on near-surface O3 columns from 900 to 700 hPa, nitrogen dioxide (NO2), and formaldehyde (HCHO), which were inferred from measurements by ozone-monitoring instruments (OMI) for 2014–2018. The nine megacities included Beijing, Tianjin, Hebei, Shandong, Shanghai, Seoul, Busan, Tokyo, and Osaka. The space-borne HCHO–to–NO2 ratio (FNR) inferred from the OMI was applied to nine megacities and verified by a series of sensitivity tests of Weather Research and Forecasting model with Chemistry (WRF-Chem) simulations by halving the NOx and VOC emissions. The results showed that the satellite-based FNRs ranged from 1.20 to 2.62 and the regimes over the nine megacities were identified as almost NOx-saturated conditions, while the domain-averaged FNR in East Asia was >2. The results of WRF–Chem sensitivity modeling show that O3 increased when the NOx emissions reduced, whereas VOC emission reduction showed a significant decrease in O3, confirming the characteristics of VOC-limited conditions in all of the nine megacities. When both NOx and VOC emissions were reduced, O3 decreased in most cities, but increased in the three lowest-FNRs megacities, such as Shanghai, Seoul, and Tokyo, where weakened O3 titration caused by NOx reduction had a larger enough effect to offset O3 suppression induced by the decrease in VOCs. Our model results, therefore, indicated that the immediate VOC emission reduction is a key controlling factor to decrease megacity O3 in East Asia, and also suggested that both VOC and NOx reductions may not be of broad utility in O3 abatement in megacities and should be considered judiciously in highly NOx-saturated cities in East Asia.

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